The volume unit of (H2 + CO) mixture per unit of electrical power in various PLS
\r\n\tThe sense of proprioception includes various aspects or submodalities such as position sense, motion sense (kinaesthesia; including the duration, direction, amplitude, speed, acceleration and timing of movements), force tension sense, and change in velocity sense.
\r\n\r\n\tProprioception is mediated by proprioceptors, a specialized subset of about 10-15% of mechanosensory neurons localized in dorsal root ganglia that convey information about the stretch and tension of muscles, tendons, joints and perhaps the skin. So, the neurological basis of proprioception originates from proprioceptors with contact specialized sensory organs in muscles (muscle spindles), tendons (Golgi tendon organs), joints (different morphotypes of sensory corpuscles including Ruffini’s corpuscles and Pacinian corpuscles) and the skin (cutaneous mechanoreceptors). Thereafter, the information originated in the proprioceptors forming complex nerve pathways reach the central nervous system at the level of the spinal cord, the cerebellum and the cerebral cortex for processing. Hence, proprioception can be regarded as a continuous loop of feedforward and feedback inputs between sensory receptors throughout the body and the nervous system.
\r\n\r\n\tIn limb and axial muscles, the proprioception originates in the muscle spindles. Nevertheless, the cephalic muscles, with the exception of the extraocular muscles and those innervated by the mandibular branch of the trigeminal nerve, lack muscle spindles. But the facial or pharyngeal proprioception plays key roles in the regulation and coordination of facial musculature and diverse reflexes. At the basis of these functional characteristics are the multiple communications between cranial nerves. Substituting muscle spindles by other kinds of proprioceptors might be at the basis.
\r\n\tOn the other hand, since the stimuli for proprioceptors are mechanical (stretch, tension, and so) proprioception can be regarded as a modality of mechanosensitivity. During the last decade progress has been made to understanding the molecular basis of mechanosensitivity. However, identity of mechanotransducers is poorly know. The mechanogated ion channels acid-sensing ion channel 2 (ASIC2), transient receptor potential vanilloid 4 (TRPV4) and PIEZO2 have been related to mechanotransduction and have been detected in proprioceptors innervating muscle spindles and Golgi tendon organs in mice. Also, mice lacking Piezo2 showed severely uncoordinated body movements and abnormal limb positions.
\r\n\tFinally, the lesion of the proprioception receptors, proprioceptors or the nerve center and pathways related to proprioception result in poor proprioception. Importantly, age-related changes also affect proprioception due to a combination of natural age-related changes to the central nervous system, nerves, joints, and muscles. Acute and long-term impairment can be related to toxicological, medical or injury conditions, but also with neuromuscular and central nervous system diseases.
\r\n\tBased on the above comments this book intends to provide a comprehensive update an overview of the anatomical, structural and molecular basis of proprioception as well as of the main causes of proprioception impairment and possible treatments.
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Vega and Dr. Juan Cobo",publishedDate:null,coverURL:"https://cdn.intechopen.com/books/images_new/10554.jpg",keywords:"Muscle Proprioception, Articular Proprioception, Sensory Receptors, Cephalic Proprioception, Primary Sensory Neurons, Spinal Cord, Cerebellum, Brain, Proprioception Impairment, Mechanosensitivity, Mechano-Gated Ion Channels, Mechanotransduction",numberOfDownloads:272,numberOfWosCitations:0,numberOfCrossrefCitations:0,numberOfDimensionsCitations:0,numberOfTotalCitations:0,isAvailableForWebshopOrdering:!0,dateEndFirstStepPublish:"September 8th 2020",dateEndSecondStepPublish:"October 6th 2020",dateEndThirdStepPublish:"December 5th 2020",dateEndFourthStepPublish:"February 23rd 2021",dateEndFifthStepPublish:"April 24th 2021",remainingDaysToSecondStep:"5 months",secondStepPassed:!0,currentStepOfPublishingProcess:5,editedByType:null,kuFlag:!1,biosketch:"Leading researcher and head of the SINPOS research group (Sensory Organs and Peripheral Nervous System), and full professor of neuroanatomy and human embryology at the University of Oviedo. 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He completed his postdoctoral training at the universities of Brno and Prague (Czech Republic), 'La Sapienza' and 'Tor Vergata' in Rome specializing in peripheral nervous system and growth factors of the neurotrophin family. Currently he is a Professor of Anatomy and Human Embryology of the Department of Morphology and Cell Biology at the University of Oviedo, and Head of the research group SINPOS (Sensory Organs and Peripheral Nervous System) at the University of Oviedo. He has taught as a contracted professor, at the Universities of Messina, 'Federico II' of Naples, Rome 'La Sapienza' and Rome 'Tor Vergata', Sassari, Barí, and CEU-San Pablo at Madrid. 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Recently, interest in hydrogen energy has increased significantly, mainly due to the energy consumption increase in the world, and recent advances in the fuel cell technology. According to the prognosis, in the next decades, global energy consumption will be increased by 59%, and still most of this energy will be extracted from the fossil fuels. Because of the traditional fossil fuels depletion, today there\'s a growing interest in renewable energy sources (f.e. – bioethanol, biodiesel). Bioethanol can be obtained from the renewable biomass, also it can be easily and safely transported due to its low toxicity, but it\'s not a very good fuel. Modern biodiesel production technologies are characterized by a high percentage of waste (bioglycerol) which is hard to recycle.
It is common knowledge [2] that addition of the syn-gas to the fuel (H2 and CO) improves the combustion efficiency: less burning time, rapid propagation of the combustion wave, burning stabilization, more complete mixture combustion and reduction of dangerous emissions (NOx). Besides, the synthesis gas is an important stuff raw for the various materials and synthetic fuels synthesizing. There are many methods of synthesis gas (including hydrogen) production, for example – steam reforming and partial liquid hydrocarbons oxidation. Also, there is an alternative approach – biomass reforming with low-temperature plasma assistance. Plasma is a very powerful source of active particles (electrons, ions, radicals, etc.), and therewith it can be catalyst for the various chemical processes activation. However, a major disadvantage of chemical processes plasma catalysis is weak processes control.
There is a bundle of electrical discharges that generate both equilibrium and non equilibrium plasma. For plasma conversion – arc, corona, spark, microwave, radio frequency, barrier and other discharges are used. One of the most effective discharges for the liquid hydrocarbons plasma treatment is the "tornado" type reverse vortical gas flow plasma-liquid system with a liquid electrode (“TORNADO-LE”) [3]. The main advantages of plasma-liquid systems are – high chemical plasma activity and good plasma-chemical conversions selectivity. It may guarantee high performance and conversion efficiency at the relatively low power consumption. Moreover, those are systems of atmospheric pressure and above, and this increases their technological advantages.
Also, syn-gas ratio – hydrogen and carbon monoxide concentration ratio should be mentioned. As well, it should be taken into consideration that for efficient combustion (in terms of energy) of the synthesis gas it should contain more hydrogen, and in the case of the synthesis materials – they should contain more CO.
Relatively new possible solution to this problem – carbon dioxide recycling. Many modern energy projects have difficulties with the large amount of CO2 storing and disposing. And it is also known that the addition of CO2 to plasma during the hydrocarbons reforming may help to control plasma-chemical processes [4]. That is why the objective of the research is to study the influence of different amounts of CO2 in the working gas on the plasma-chemical processes during the hydrocarbons conversion.
This research deals with hydrocarbons (bioethanol, bioglycerol) reforming by means of the combined system, which includes plasma processing and pyrolysis chamber. As a plasma source the "tornado" type reverse vortical gas flow plasma-liquid system with liquid electrode has been used [5].
Qualitatively new challenge is connected with a selectivity of the plasma chemistry strengthening by the transition of the chemical industry to "green chemistry". The last is a transition from the traditional concept of evaluating the effectiveness of the chemical yield to the concept that evaluates the cost-effectiveness as the exclusion of hazardous waste and non-toxic and/or hazardous substances [6].
A quantitative measure of the environmental acceptability of chemical technology is the ecology factor, which is defined as the ratio of the mass of waste (waste) to the mass of principal product. Waste is all that is not the principal product.
By the way, the most promising approaches in green chemistry is the implementation of processes in supercritical liquids (water, carbon dioxide) [7].
Water in supercritical condition unlimitedly mixes with oxygen, hydrogen and hydrocarbons, facilitating their interaction with each other - oxidation reactions are very fast in scH2O (supercritical water). One particularly interesting application of this water - efficient destruction of chemical warfare agents. When mixed with other substances scH2O can be used not only for oxidation but also in the reactions of hydrolysis, hydration, the formation and destruction of carbon-carbon bonds, hydrogenation, and others.
Besides, the use of pulsed electrical discharges in the liquid brings up new related factors: strong ultraviolet emission and acoustic or shock waves. In literature it can be found that systems with energies more than 1 kJ/pulse, that have negative influence on the lifetime of such systems. Reasonable from this perspective is the usage of pulsed systems with relatively low pulse energy and focusing of acoustic waves. In addition, the acoustic oscillations in such systems can be used as an additional mechanism of influence on chemical transformations.
In using of acoustic oscillations for chemical reactions the most attention is paid to systems with strong convergent waves. However, the processes during the collapse of the powerful convergent waves are studied unsufficiently. In the literature the systems of cylindrical, spherical or parabolic surfaces used in the focusing of shock waves for technological needs are known [8]. However, among their disadvantages should be noted that partial usage of the energy of acoustic wave and the problem of it’s peripheral sources synchronization, which leads to distortion of the shock wave front ideality and reduces the focusing effectiveness.
Probably, more perspective method of using acoustic waves is their generation by single axial pulse electric discharge with further reflection from an ideal cylindrical surface. This approach can provide better symmetry of compression by convergent acoustic wave both in the gas and in the liquid. Probably, such mechanism can be exploited for scH2O production
In addition, the re-ignition of electrical discharge at the moment of collapse convergent acoustic waves can lead to the plasma temperature increasing due to compression of the discharge channel, as well as the appropriate amplification of acoustic waves after the collapse.
It\'s clear that plasma-liquid systems (PLS) mentioned above have some sharp differences. Therefore, the first section of this article presents the results of our research on the addition of CO2 to the “TORNADO-LE”. And the second section of the article is devoted to investigation of double-impulse system in underwater electric discharge.
The experimental setting is shown in Fig. 1. Its base is a cylindrical quartz chamber (1) with diameter of 90 mm and height of 50 mm. Top (2) and bottom (3) it is hermetically closed with metal flanges. Camera is filled with fluid (4), the level of which has been maintained by the injection pump through the hole (5). Bottom flange is made of stainless steel. The stainless steel T-shaped cylindrical electrode (6), cooled with water, immerses in the liquid through the central hole in the bottom flange. There is a 5 mm thick metal washer on its surface (7) in the middle of which there is a hole in diameter of 10 mm. Sharp corners are rounded. This washer is used for reducing the waves (which have been moving to the quartz wall) amplitude on the liquid surface.
The top flange, made from duralumin, contains copper sleeve (13) with a diameter of 20 mm is placed in the center (2), and plays the role of the second electrode. The nozzle with diameter of 4 mm and length of 6 mm is located in the center of the copper sleeve (8). Gas is introduced into the flange (2) through the aperture (9). Gas flow changes the direction at 90 degrees inside the flange and injects tangentially into the channel (10). (10) The gas is rotated in the circular channel. Rotating gas (11) lands on the surface liquid and moves to the central axis of the system, where fells into the quartz cell through the nozzle (14), forming a plasma torch (12). Camera (14), in its turn, plays a role of pyrolytic chamber. Flow rate reaches the maximum value near the nozzle. Due to this, the zone of lower pressure is formed in the center of the gas layer, compared to the periphery. The conical structure appears over the liquid’s surface near the system axis (Fig. 1). External static pressure is 1 atm. and internal - 1.2 atm (during discharge burning). Gas from quartz chamber (14) gets into the refrigerator (15), which is cooled with water at room temperature.
Schematic set up of the “TORNADO-LE”.
Condensed matter (16) together with the gas from the refrigerator gets to the chamber (17). At the chamber exit (17) there\'s a flask (18), where gas is gathered for its composition diagnostics by means of mass spectrometry and gas chromatography. Study of plasma parameters is performed by emission spectrometry. The emission spectra registration procedure uses the system which consists of optical fiber, the spectral unit S-150-2-3648 USB, and the computer. Fiber is focusing on the sight line in the middle between the top flange (2) and the surface of the liquid (4).
The spectrometer works in the wavelength range from 200 to 1100 nm. The computer is used in both control measurements process and data processing, received from the spectrometer.
The voltage between the top flange and electrode, immersed in the liquid, is supplied by the power unit "PU". DC voltage provided is up to 7 kV. Two modes of operation have been considered:
"liquid" cathode (LC) – electrode immersed in the liquid has "minus" and the top flange has "plus";
solid" cathode (SC) - with the opposite polarity.
Electrode which has "plus" is grounded. Breakdown conditions are controlled by three parameters: the fluid level, the gas flow value and the voltage magnitude between the electrodes. The several modes of operation have been studied:
Various air flow and CO2 ratio;
Discharge voltage varied within Ud = 2.2 ÷ 2.4 kV;
Discharge current varied within Id = 220 ÷ 340 mA (ballast resistance hasn’t been used).
At first, for the analysis of the plasma-chemical processes kinetics the distilled water (working fluid), and ethanol (ethyl alcohol solution in distilled water with a molar ratio C2H5OH/H2O = 1/9.5), as a hydrocarbon model have been used. As the working gas mixture of air with CO2, in a wide range of air flow and CO2 ratios has been used. The ratio between air and CO2 in the working gas changes in the ranges: CO2/Air = 1/20 ÷ 1/3 for the working fluid C2H5OH/H2O (1/9.5) and CO2/Air = 0/1 ÷ 1/0 (by pure air to pure CO2) - for distilled water.
Plasma component composition and population temperature of the excited electron (Te*), vibration (Tv*) and rotational (Tr*) levels of plasma components and relative concentrations of these components have been determined by the emission spectra. For the temperature population determination of the excited oxygen atoms electron levels the Boltzmann diagram method has been used [5]. Te* of oxygen atoms has been determined for the three most intense lines (777.2 nm, 844 nm, 926 nm). Temperature population of excited hydrogen atoms electron levels has been determined by the two lines of 656.3 nm and 486 nm relative intensities.
The effect of the presence of CO2 in the system on the initial gas products has been investigated by means of “TORNADO-LE” current-voltage characteristics with changes in the working gas composition. Tv* and Tr* have been determined by comparing the experimentally measured emission spectra with the molecules spectra simulated in the SPECAIR program [9]. With help of this program and measured spectra, relative component concentrations in plasma have been determined. Also, the concentration of atomic components has been obtained by calculating the amount of oxygen that fell into a working system with the working gas flow. The hydrogen amount has been received from the electrolysis calculations. The output gas in reforming ethanol has been analyzed by gas chromatography and infrared absorption.
The process of discharge ignition occurred as follows: the chamber is filled with liquid to a fixed level (5 mm above the washer). At the next stage a certain amount of gas flow forms the stationary cone from liquid; the voltage applied between the top flange and electrode immersed in a liquid starts gradually increase. When the voltage reaches a break-out value - Ub, a streamer appears for the first time. After that, burning discharge starts in split second, and then voltage decreases and current increases. After a second or two it is stabilized. During this time – static pressure rises inside the chamber from 1 to 1.2 atm. If you maintain the liquid level fixed, then the discharge is quite steady.
Liquid layer thickness of 5 mm has been chosen because that is the minimum liquid thickness in which the discharge burns between the liquid surface and the top flange. If the thickness is smaller plasma pushes the water toward the electrode immersed in the liquid and the discharge starts burning between two metal electrodes. Discharge goes into the arc regime. When the thickness of the distilled water layer above the washer is 5 mm (in the case of air flow only) break voltage reaches 4.5 kV and for a CO2 flow - 6 kV. It is known [10], this increase in break-out voltage derives from the appearance of an additional loss channel of electrons – due to their sticking onto CO2 molecules. This sticking has dissociative character and it is accompanied by the energy expense.
For example, the threshold reaction with CO2 is 3.85 eV. Therefore CVC in pure CO2 is decreased (Fig. 2). When the thickness of the С2Н5ОН/H2O (1/9.5) solution layer above the washer is 5 mm (in the case of air flow only) the break voltage is 5.5 kV, and for the air flow mixture with CO2 (CO2/Air = 1/3) – 6.5 kV. Adding CO2 to the air leads to the increase in the break-out voltage value. Adding ethanol to distilled water (С2Н5ОН/H2O = 1/9.5) results in the increase of break voltage on 1 kV. Power supply unit provides maximum voltage of 7 kV. Increasing the thickness of the fluid layer above the washer (> 5 mm) leads to the increase of the break-out voltage value. There is no discharge ignition with a break-out voltage value of more than 7 kV. Therefore, 5 mm thickness of the liquid layer above the surface immersed in a liquid metal electrode (washer) has been chosen as the optimum one.
The current-voltage characteristics of the discharge are shown for the SC mode (Fig. 2 a; 2b). The cell has been filled with distilled water (Fig. 2a) or bioethanol (Fig. 2b).
a) Current-voltage characteristics of the discharge at different ratios of CO2/Air in the working gas. Working liquid - distilled water. Airflow - 55 and 82.5 cm3/s, the flow of CO2 - 4.25, 8.5 and 17 cm3 /sec. b) Current-voltage characteristics of the discharge at the ratio CO2/Air = 1/5 in the working gas. Working liquid – С2Н5ОН/H2O (1/9.5) solution. Airflow - 82.5 cm3/s, the flow of CO2 - 17 cm3/s.
The "tornado" type reverse vortex gas flow is formed by gas flow, which is a mixture of air with СО2 in varying proportions. Ratio of CO2/Air is changed in the range from 1/20 to 1/3, and in the case of ethanol and 1/0 in the case of water. Current varied in the range from 230 to 400 mA. The initial level of the working liquid is the same in all cases.
The current-voltage characteristics show that adding a small amount of СО2 (near 20%) to the working gas has no effect on the discharge type in various studied working liquids. In the range of flow ratios CO2/Air from 1/20 to 1/5 characteristics are straight lines. It was observed that the increasing of СО2 share in working gas causes discharge voltage supply rise.
Typical emission spectra of the plasma are shown in Fig. 3a and Fig. 3b for the cases with the distilled water as the working liquid and the solution of С2Н5ОН/H2O (1/9.5).
The emission spectra show that when the working liquid is distilled water, plasma contains the following components: atoms H, O, and hydroxyl OH. In case when the working liquid is С2Н5ОН/H2O solution (1/9.5), plasma has the following components: atoms – N, O, C, Fe, Cr, molecules – OH, CN, NH. The emission spectra shows that the replacement of the working liquid with distilled water with ethanol CN and lower electrode material made of stainless steel (anode) occur in plasma. Occasionally, during discharge burning breakdown may occur in С2Н5ОН/H2O layer solution (1/9.5).
Those breakdowns may occur due to the fact that during the discharge burning, thickness of liquid layer, when the working fluid has a significant share of С2Н5ОН, a current channel is formed through the liquid layer to the metal electrode. And in the case of distilled water - plasma channel discharge ends near the surface of the liquid. It may indicate the presence of large liquid surface charge.
It was observed that the increase of CO2 in the working gas (CO2/air > 0.3) leads to an increase in the intensity of hydrogen and oxygen radiation lines (H and O) at the time when the intensity of the molecular component (OH) radiation, within the error, is stable (I = 300 mA, U = 1.9-2.4 kV, air flow 0 - 82.5 cm3/sec, the flow of CO2 - 4.25 - 85 cm3/sec).
a) Emission spectrum of the plasma in TORNADO-LE plasma-liquid system, where the working liquid is distilled water. Working gas - a mixture of СО2/air = 1/0, Id = 300 mA, U = 2.2 kV, the flow of CO2 - 85 cm3/s and СО2/air = 1/20, Id = 300 mA, U = 1.9 -2.0 kV, air flow - 82.5 cm3/s, the flow of CO2 - 4.25 cm3/s. b) Emission spectrum of the plasma in the TORNADO-LE plasma-liquid system, where the working fluid is bioethanol. Working gas - a mixture of СО2/air = 1/20, Id = 300 mA, U = 2 kV, air flow - 82.5 cm3/sec, the flow of CO2 - 4.25 cm3/sec.
Fig. 4 shows the ratio of the hydrogen (Hα λ = 656.3 nm) and oxygen (O, λ = 777.2 nm) radiation intensity to the highest point of band hydroxyl (OH, λ = 282.2 nm) small intensity at different ratios of CO2/air (I = 300 mA, U = 1.9 – 2.4 kV, air flow - 27.5, 55 and 82.5 cm3/s, the flow of CO2 - 4.25, 8.5, 17, 42.5 and 85 cm3/s). High intensity bands haven\'t been used in the calculations because of the possible reabsorption. (I = 300 mA, U = 2 – 2.2 kV). In the case of distilled water (Fig. 4a), results are presented for the three air flows - 27.5, 55 and 82.5 cm3/s and five CO2 streams - 4.25, 8.5, 17, 42.5 and 85 cm3/s (I = 300 mA , U = 1.9 – 2.4 kV). Air and CO2 flows are variated so that the total flow compiles similar values and achieves ratios of CO2/air in a wide range from 1/20 to 1/0.
The ratio of the radiation intensity of hydrogen (Hα λ = 656.3 nm) and oxygen (O, λ = 777.2 nm) to the peak of the band hydroxyl (OH λ = 282,2 nm) at different ratio CO2/Air in the working gas. Working liquid - distilled water (a) I = 300 mA, U = 1.9 – 2.4 kV and bioethanol (b) I = 300 mA, U = 2 -2.2 kV.
In calculating the relative concentration ratio of hydrogen to oxygen from the emission spectra, it was observed that the hydrogen concentration is two times as much of the oxygen concentration for the case of distilled water as the working liquid - (I = 300 mA, U = 1.9 – 2.4 kV, airflow - 27.5, 55 and 82.5 cm3/sec, the flow of CO2 - 4.25, 8.5, 17, 42.5 and 85 cm3/sec), and ten times as much when the working liquid is С2Н5ОН/H2O solution (1/9.5) (I = 300 mA, U = 2 - 2.2 kV, air flow - 55 and 82.5 cm3/sec, the flow of CO2 - 4.25, 8.5 and 17 cm3/sec). However, according to the calculations, these components production by means of electrolysis and their extraction from the working gas, the oxygen concentration exceeds the average hydrogen concentration in three orders of magnitude, unless the case when the pure CO2 is used as a working gas.
It should be noted that the addition of CO2 reduces the discharge stability, especially in the case of bioethanol. In determination of the temperature population excited electron levels of plasma atomic component the most intense lines (spectra with the smallest possible accumulation in the experiment measurement of 500 ms) have been used, according to the discharge burning particularity. Also, it affects the parameters determination accuracy.
Temperature of excited hydrogen electron population levels is determined by the relative intensities (two lines of 656 nm and 486 nm). For the case where the working liquid is distilled water –
Temperatures of OH excited vibrate and rotational population levels have been determined by comparing the experimentally measured emission spectra with the molecular spectra modeled in The SPECAIR program. In the case when the working liquid is distilled water, appropriate temperatures are:
During the study, it turned out that the addition of CO2 weakly affects the population temperature of excited electron, vibration and rotational levels of plasma components (Fig. 5) (I = 300 mA, U = 1.9 - 2.4 kV, air flow - 27.5, 55 and 82.5 cm3/s, the flow of CO2 - 4.25, 8.5, 17, 42.5 and 85 cm3/s). Weak tendency to temperature decrease has been observed, but these changes do not exceed the error.
Population temperatures of excited electron, vibration and rotational levels of plasma components at different ratio of CO2/Air in the working gas. Working liquids - distilled water (a) and ethanol (b)
Fig. 6–7. shows the results of gas chromatography bioethanol conversion output products. Results are presented for two air streams 55 and 82.5 cm3/s + three CO2 streams: 4.25, 8.5 and 17 cm3/s (I = 300 mA, U = 2 – 2.2 kV). CO2/Air ratio in the range from 1/20 to 1/3 has been changing exactly this way. Selection of gas into the flask has been taken place at the refrigerator output. The flask has been previously pumped by the water-jet pump to the pressure of saturated water vapor (23 mm Hg).
Fig. 6 shows the gas chromatography comparison of bioethanol conversion output products with and without the addition of CO2. The air flow is constant – 55 cm3/s, in case of CO2/Air = 1/3 – 17 cm3/s of CO2 has been added to the air (the total flow has been increased, which may explain the decrease in the percentage of nitrogen at a constant air flow; I = 300 mA, U = 2 - 2.2 kV). This histogram shows that adding of carbon dioxide leads to a significant increase of the H2 component percentage, CO (syn-gas) and CH4 in the output gas. This may indicate that the addition of CO2 during the ethanol reforming increases the conversion efficiency, because CO2 plays a burning retarder role.
Gas chromatography comparison of bioethanol conversion output products with and without the addition of CO2.
Gas chromatography comparison of bioethanol conversion output products by adding different amounts of CO2.
The ethanol solution consumption for the SC mode with current of 300 mA and air flow of 55 cm3/ equals 6 ml/min, and for the air flow of 82.5 cm3/s and CO2 of 17 cm3/s mixture - 10 ml/min.
According to the gas chromatography, in the studied correlations range of CO2/Air, syn-gas ratio ([H2]/[CO]), changes slightly – look at Fig. 8. Measurements were made by two air streams of 55 and 82.5 cm3/s and three CO2 streams of – 4.25, 8.5 and 17 cm3/s; I = 300 mA, U = 2 – 2.2 kV.
Syn-gas ratio of bioethanol conversion output products for various ratios of CO2/Air in the range between 0/1 - 1/3.
Besides the gas chromatography, the output gas composition has been studied by means of infrared spectrophotometry (IRS). Fig. 9 shows a typical IRS spectrum of the output gas. In the SC mode (current 300 mA, voltage 2 kV) the working liquid is ethyl alcohol and distilled water mixture (С2Н5ОН/H2O = 1/9.5), and the working gas – air (82.5 cm3/s) and CO2 (4.25 cm3/s) mixture. Research has been carried out in a ditch with a length of 10 cm and a diameter of 4 cm. Pressure inside the ditch has been 1 atm. The ditch walls have been made of BaF2.
Fig. 10 shows the dependence of the CO transmission standardized maximum intensity peaks (2000 - 2250 cm-1) in the syn-gas, depending on the CO concentration according to gas chromatography results. Standardization has been conducted for the maximum intensity value of the CO transmission peak bandwidth at the SC mode with the current of 300 mA, voltage - 2 kV, the mixture of ethyl alcohol and distilled water (С2Н5ОН/H2O = 1/9.5) as the working liquid, and the mixture of air (82.5 cm3/s) and CO2 (4.25 cm3/s), as the working gas.
According to IR spectrophotometry CO fraction in the synthesis gas is practically the same. According to gas chromatography CO fraction in the synthesis gas in the different operation modes stays on the same level as well (the changes are in the range of 1%). So IR spectrophotometry can be used determine the composition of synthesis gas under ethanol reforming.
The SC mode (current 300 mA, voltage 2 kV) the working liquid is ethyl alcohol and distilled water mixture (С2Н5ОН/H2O = 1/9.5), the working gas – air (82.5 cm3/s) and CO2 (4.25 cm3/s) mixture
Dependence of the normalized maximum intensity peaks (2000-2250 cm-1) transmission of CO in the syn-gas, depending on the concentration of CO according to gas chromatography data.
Plasma provides gas generation, which contains a certain amount of the syn-gas. The energy needed for this plasma support (Qp) has been calculated by the following formula:
where Pd - power that has been embedded into the discharge, t – production time of gas volume unit during the reforming process. Electrical energy transformation coefficient α has been calculated by the formula:
where Qs - energy that is released during the complete combustion of syngas (obtained in the reforming process).
Electrical energy transformation coefficient α has value of 0.81 for the "TORNADO-LE" with an ethanol solution and pure air flow 55 cm3/s. And the CO2 addition (the ratio of CO2/air = 1/3) gives the value of α = 1,01. System electrical parameters are as follows: I = 300 mA, U = 2 – 2.2 kV.
In the model of calculations was assumed that the discharge is homogeneous over the entire volume. It is justified at zero approximation, because the time of gas mixing in the radial direction is less than the times of characteristic chemical reactions. Also we neglect the processes in the transitive zone between the discharge to post-discharge. Thus, the time of gas pumping through the transition region is too short for the chemical reactions to have a sufficient influence on the concentration of neutral components.
The total time of calculation is divided into two time intervals: the first one is the calculation of the kinetic processes of fast generation of active atoms and radicals in the discharge region. Those components accelerate the formation of molecular hydrogen, carbon oxides and production of other hydrocarbons. The second time interval is the oxidation of the gas mixture in the post-discharge region as a result of the high gas temperature and the presence of O and OH. These components remain in the mixture after the dissociation of water and oxygen molecules by electron impacts in the plasma. The oxidation of generated hydrocarbons has a noticeable influence on kinetics in the investigated mixture due to the high gas temperature.
Under the aforementioned conditions, the characteristic time of oxidation is approximately equal to the air pumping time through the discharge region (~10−3–10−2 s). The following system of kinetic equations is used in order to account for the constant air pumping through the system:
Ni, Nj, Nl in the equation (3) are the concentrations of molecules and radicals; kij, kiml are the rate constants of the processes for the i-th component. The rates of electron–molecule reactions Sei are connected with discharge power and discharge volume. The last three terms in equation (1) describe the constant inflow and outflow of gas from the discharge region. The term Ki is the inflow of molecules of the primary components (nitrogen, oxygen, carbon dioxide, water and ethanol) into the plasma, G/VNi and kNi are the gas outflow as the result of air pumping and the pressure difference between the discharge region and the atmosphere. In order to define the initial conditions, the ethanol/water solution is assumed to be an ideal solution. Therefore, the vapor concentrations are linear functions of the ethanol-to-water ratio in the liquid. The evaporation rates Ki of C2H5OH and H2O are calculated from the measured liquids’ consumption. The inflow rates Ki of nitrogen and oxygen are calculated by the rate of air pumping through the discharge region:
where N0i correspond to [N2] and [O2] in the atmospheric pressure air flow.
The gas temperature in the discharge region is taken to be constant in the model. In reality, the gas temperature T is dependent on the gas pumping rate and the heat exchange with the environment. Therefore, in order to take into account those influences, T is varied in the interval 800–2500K (similarly to the experimentally obtained temperature spread). After ~10−2 s, the balance between the generation and decomposition of the components leads to saturation of concentrations of all species. This allows us to stop the calculations in the discharge region and to investigate the kinetics in the post-discharge region. System (3) is solved without accounting for the last three terms on the time interval without the plasma. The calculations are terminated when the molecular oxygen concentration reaches zero level.
The full mechanism developed for this experimental work is composed of 30 components and 130 chemical reactions between them and its closed to [11]. The charged particles (electrons and ions) are ignored in the mechanism, because of low degree of ionization of the gas (~ 10−6 – 10−5). Nitrogen acts as the third body in the recombination and thermal dissociation reactions. In the non-equilibrium plasma almost the entire energy is deposited into the electron component. The active species, generated in the electron–molecular processes, lead to chain reactions with ethanol molecules.
Numerical simulation of kinetics showed that the main channels of H2 generation in the plasma were ethanol abstraction for the first 10–100μs, and hydrocarbon abstraction afterwards. Additionally, the conditions when the reaction between H2O and hydrogen atoms was the main channel of H2 production were found. A kinetic mechanism, which adequately described the chemistry of the main components, was proposed. The model did not account for nitrogen-containing species, and nitrogen was considered only as a third body in recombination and dissociation reactions. The comparison between experiments and calculations showed that the mechanism can adequately describe the concentrations of the main components (H2, CO, CO2, CH4, C2H4, C2H6, and C2H2).
However, it should be noted that with the increase in temperature to 2523 K leads to the fact that the output of the reactor is not observed almost no light hydrocarbons. They simply "fall apart" and burned. That leaves the most stable elements such as H2O, N2, CO2. This suggests that the increase in temperature up to these values is not advisable because of the decrease in the yield of useful products (see Fig. 11 and Fig. 12a,b).
The dependence of the reaction main products of the flow rate of CO2 (inside discharge), T = 2023 K
a). The dependence of the reaction main products of the flow rate of CO2 (after discharge), T = 2023 K. b). The dependence of the reaction main products of the flow rate of CO2 (after discharge), T = 2023 K
These calculations are based in good correspondence with the experimental data (see Fig. 8).
Other model hydrocarbon is bioglycerol (crude glycerol) which is a byproduct of the biodiesel manufacture. Biodiesel is a popular alternative fuel. It is carbon neutral, has emissions equivalent or below diesel, is biodegradable, non-toxic, and is significantly cheaper to manufacture than its petroleum equivalent. However there is one significant drawback: for every 10 gallons of biodiesel produced, roughly 1 gallon of bioglycerol is created as a byproduct.
Biodiesel is produced by mixing vegetable oil and potassium hydroxide KOH. Therefore, the large-scale production of environmentally friendly and renewable fuel may lead to possible bioglycerol accumulation in large quantities, which, in turn, can cause environmental problems, as it is comparably bad fuel. In addition, it has a rather large viscosity of 1.49 Pa•s, which is larger for almost three orders of magnitude than ethanol and water viscosity. The solution to this problem would be "TORNADO-LE" usage for bioglycerol reforming. Pure glycerol chemical formula is C3H5(OH)3. However, bioglycerol contains various impurities (including a set of alkali).
Fig. 13 shows a photograph of burning discharge, where the working liquid is bioglycerol and working gas - air. Research is conducted by the SC polarity, because this mode has lowest liquid consumption.
Photo of the combustion discharge in which the working liquid is bioglycerol and working gas - air.
Fig. 14 shows the typical emission spectrum of the plasma discharge in a "TORNADO-LE" where the working liquid is bioglycerol doped with alkali. It is registered at a current of 300 mA, voltage – 2 kV, air flow – 110 cm3/s. Optical fiber is oriented on the sight line, parallel to the liquid surface in the middle of the discharge gap. The distance from the liquid surface to the top flange equals 10 mm.
Emission spectrum (Fig. 14) is normalized to the maximum Na doublet (588.99 nm, 589.59 nm). It contains K (404.41 nm, 404.72 nm, 766.49 nm, 769.89 nm), Na (588.99 nm, 589.59 nm), Ca (422.6 nm) lines, and a part of continuous spectrum, which indicates that the there\'s a soot in the discharge. Temperature, which is defined by the plasma continuous emission spectrum is 2700 ± 100 K.
Typical emission spectrum of the plasma discharge, which burns in a mixture of air and bioglycerol / alkali.
The K, Na, Ca elements presence in the discharge gap complicates the plasma kinetics numeric modeling of the bioglycerol reform process. The gas flow rate at the system outlet is 190 cm3/s, i.e. by 80 cm3/s larger than the initial (110 cm3/s), which indicates bioglycerol reforming to the syn-gas. Liquid flow is 5 ml/min. Change of the CO2 share in the working gas weakly affects the spectrum appearance.
Based on the continuous nature of the plasma emission spectra, we compared the experimental results with the calculated spectra of the blackbody radiation. Calculations have been performed by using Planck\'s formula.
Fig. 15 shows the computational grid with step of 200-300 K in the temperature range from 2500 K to 3500 K and the plasma emission spectrum in the case of bioglycerol, as a working fluid (air flow - 82.5 cm3/s, the flow of CO2 - 17 cm3/s, CO2/Air = 1/5, Id = 300 mA, U = 600 V). All spectra are normalized to the intensity, which is located at a wavelength of 710 nm.
Plasma emission spectrum in the case when the working gas is a mixture SO2/Air = 1/5 (air flow - 82.5 cm3/s, the CO2 flow - 17 cm3/s), Id = 300 mA, U = 600 V and calculated spectra of blackbody radiation)
The data in Fig. 15 show that the plasma emission spectrum coincides with the calculated by the Planck formula for the temperature T = 2800 ± 200 K. Since bioglycerol contains alkali metals, which represent an aggressive environment, the gas chromatography can\'t be used. Therefore, in order to determine the gas composition, formed the bioglycerol reformation IR and mass spectrometry have been used.
With infrared transmission spectra one can see that the transition to bioglycerol increases the amount of such components as CO2 (2250-2400 cm-1), CO (2000-2250 cm-1), CH4 (3025-3200 cm-1), C2H2 (3200-3350 cm-1).
Electrical energy is added to the “TONADO-LE” plasma-liquid system in the form of plasma power. Plasma acts as a catalyst and thus this power should be controlled. In addition to electric energy for plasma we incorporate hydrocarbon (ethanol or bioglycerol) as an input to the system. These hydrocarbons are raw material for syn-gas generation but they are also a fuel which has some energy associated with it. So, we input some energy to the system (hydrocarbon + electricity) and we get syn-gas, which is potentially a source of energy as well.
Carbon dioxide adding leads to a significant increase the percentage of H2 + CO (syn-gas) and CH4 components in the exhaust. This may indicate that the CO2 addition under the ethanol reforming increases the conversion efficiency, because CO2 plays a role of the retarder in the system by reducing the intensity of the conversion components combustion.
The transmission spectra of infrared radiation indicate that the exhaust gas obtained by ethanol solution conversion, contains such components as CO, CO2, CH4, C2H2. It was found that CO2 adding reduces the CH4 and C2H2 amount, but does not affect the amount of producted CO.
The possibility of hydrocarbons reforming, which have considerable viscosity (bioglycerol) in the "TORNADO-LE" is shown. This gives a possibility to avoid environmental problems due to the bioglyсerol accumulation during biodiesel production.
The α coefficient [see (2)] in bioglycerol reforming is higher than ethanol reforming at the same ratios of CO2/Air in the input gas. This may be connected with the lower power consumption on the plasma generation in case of bioglycerol reforming. Bioglycerol contains alkaline dash, which increases the bioglycerol conductivity. Bioglycerol reforming products contain mainly CO and hydrocarbons CH4, C2H2, which also gives some contribution to energy yield.
The experimental setting is shown in Fig. 16. The main part of the system is cylinder with height H = 10 mm, and radius R = 135 mm. Its lateral surface made of stainless steel with a thickness of 5 cm. This cylinder is filled with liquid for experimental operations. The electrodes are placed perpendicular to the cylinder axis. They have the diameter of 10 mm, made of brass, and their ends are shaped hemispheres with a radius of curvature of 5 mm. The discharge (2) is ignited between the rounded ends of the electrodes. At a distance of 40 mm from the lateral surface of the cylinder is piezo-ceramic pressure sensor (3), which records acoustic vibrations in the fluid, caused by electric discharge under water. The distance between the sensor head and the system axis = L.
Schematic diagram of plasma-liquid system with a pulsed discharge, 1 - electrodes with brass tips, 2 – plasma, 3 – piezo-ceramic pressure sensor.
The cylindrical system could be located in a horizontal position (Fig. 17a) or vertical one (Fig. 17b). The full volume (0.5 l) of system is fluid-filled. The fluid in the system can be processed as in static mode (no flow), and dynamic one (with flow ~ 15 cm3/s). Additional supply of gas may be realized in the system also (airflow ~ 4 cm3/s), which is injected through a spray nozzle (source diameter 8 mm) located near the inner wall of the cylinder at a distance of 130 mm from the discharge gap (Fig. 16). The working fluids are: the tap water (with and without flow), distillate and ethanol (96%, no flow).
The main feature of electrical scheme for pulsed power feeding of discharge in a liquid is usage of two independent capacitors which are supplied two independent sources of power (1 kW). Pulsed discharge realized in two modes: single and double pulses. In the single pulse mode only one capacitor is discharged with a frequency of 0 - 100 Hz.
Double pulse mode is realized as follows: one capacitor discharges in the interelectrode gap through air spark gap; the clock signal from the Rogowski belt after first breakdown is applied to the thyratron circuit and second capacitor discharges through it. This set of events leads to the second breakdown of the discharge gap and second discharge appearance.
Delay of the second discharge ignition may be changed in range of 50 - 300 microseconds. The following parameters are measured: discharge current and the signal from the pressure sensor. The Rogowski belt has the sensitivity 125 A/V, and its signal is recorded with an oscilloscope. Capacity for the first discharge (C1) = 0.105 μF and it is charged to U1 = 15 kV (energy E1 = 12 J), capacity for the second discharge C2 = 0.105 µF and it is charged to U2 = 18 kV (energy E2 = 17 J).
A distance between electrodes can be changed in the range of 0.25 - 1 mm. The second discharge can be ignited at the moment (according to the delay tuning) when the reflected acoustic wave, created by the first electric discharge in liquid, returns to the center of the system (the time of its collapse ~ 180 ms).
Photograph of the cylinder from the outside: a) horizontal position, b) vertical position.
The composition of ethanol and bioethanol reforming products is studied with gas chromatography, in case of bioglycerol reforming - mass spectrometry and infrared spectrophotometry.
Oscillograms of current and acoustic signal for different distances between electrodes (0.5 and 1 mm) are presented in Fig. 18. These oscillograms show the presence of electrolysis phase before breakdown, while duration of electrolysis increases with interelectrode distance.
Oscillograms of the discharge current (top curve) and signal piezo-ceramic pressure sensor (lower curve): a) d = 0.5 mm, b) d = 1 mm. Tap water flow = 15 cm3/sec, without the input gas stream, C = 0.18 uF, U = 13.5 kV; ballast resistor in the discharge circle: Rb = 20 Ohm, the cylinder is in horizontal position.
Oscillograms of current and acoustic signal in the single pulse mode at the different discharge ballast resistor: Rb: a) - 0 Ohm, b) - 10 Ohm; c) - 20 Ohm, d) - 50 Ohm. Tap water flow 15 cm3/s, without the input gas stream, d = 0.5 mm, C = 0.015 µF, U = 19.5 kV, the cylinder is in horizontal position.
Fig. 19 shows the acoustic signal dependence from ballast resistor in the discharge electric circuit. The acoustic signal has two splashes: №1 - the first diverging acoustic wave, and №2 - the second diverging acoustic wave. When the ballast resistor is increased, first and second acoustic signal splashes are decreased. This may be due to the fact: we increase the ballast resistor and set measures to the discharge current, as a result the injected into the discharge gap energy is diminished.
Also, there is a signal immediately behind the front of the first splash, which is founded in all cases at 110 microseconds interim from the beginning of the discharge current. The acoustic wave passes the way near 17 cm during this time. The pressure sensor is located at the distance of 2 cm from the lateral surface, so the acoustic signal passes the way near 12 cm to the sensor. Thus, there is a second stable signal after the first splash through time ~ 29 µs, which corresponds to the path ~ 4.4 cm, so the signal can be the convergent acoustic waves reflected from the wall.
Oscillograms of the discharge current (top oscillogram) and acoustic signal (lower oscillogram) at different delays of the second discharge pulse.
There is the third acoustic signal splash in the experiment, but it does not affect the second discharge pulse delay in relation to the first. In addition, there is no acoustic signal from to the second discharge pulse in the double pulse mode, although the single pulse signal is present in the single pulse mode (Fig. 20).
Oscillograms of the discharge current (top oscillogram) and the acoustic signal (lower oscillogram) in the single pulses mode. Working fluid - ethanol, d = 0.25 mm, C1 = 0.105 µF, U1 = 15 kV, the cylinder in the vertical position
Fig. 21 shows clearly that the duration and amplitude parameters for the first current pulse in the ethanol are virtually indistinguishable from the first current pulse in distilled water at any cylinder orientations. The ratio of the second acoustic signal amplitude to the first acoustic signal amplitude in the ethanol is noticeably less than in the tap water and distillate.
The results of oscillographic studies of the discharge current and acoustic signals in double pulses mode demonstrate that the first discharge in double pulses mode takes place in the narrow gas channel with a radius comparable to the size of the plasma channel, and the second discharge takes place in the wide channel with radius larger than the plasma channel.
Next, we present the results of ethanol reforming studies in the impulse plasma-liquid system with double pulses mode and their comparison with the results obtained for "TORNADO-LE".
The mass spectrometer studies of ethanol reforming in the impulse PLS of cylindrical geometry were carried out in the following modes: single pulse mode (C = 0.105 µF, U = 15 kV, f = 15 Hz, power 180 W) and double-pulse mode (C1 = C2 = 0.105 µF, U1 = 15 kV, U2 = 15 kV, f = 15 Hz, second pulse delay = 170 µs, this time is less on 10 µsec than collapse time, the power is 435 Wt), the interelectrode distance - 0.25 mm, working liquid - ethanol (96%), the input airflow is 4 cm3/s.
Mass spectrum for double pulse mode. Ethanol is without flow, inlet gas stream - 4 cm3/s, d = 0.25 mm, C1 = C2 = 0.105 µF, U1 = 15 kV, U2 = 18 kV, the cylinder is in the vertical position, f = 15 Hz.
Mass spectrum for the single pulse mode. Ethanol without flow, inlet air flow - 4 cm3/s, d = 0.25 mm, C1 = 0.105 µF, U1 = 15 kV, the cylinder is in the vertical position, f = 15 Hz.
The mass spectrometric studies show that the main components of the output fuel mixture are: hydrogen, carbon dioxide, and molecular nitrogen. The values of these components in the mixture: H2 - 29%, CO - 17% for double pulse mode and H2 - 35%, CO - 7% for single pulse mode. That is, with the same molecular hydrogen output, the carbon dioxide yield is significantly increased in double pulses mode.
The typical mass spectrum (Fig. 24) of the ethanol reforming (ethanol aqueous solution ethanol with concentrations 3.5, 13 and 26 percents) in the "TORNADO-LE". The power is 640 Wt. It is injected in the plasma for its generation, and inlet air flow is 55 cm3/s.
Mass spectrum of the output mixture in the ethanol reforming (ethanol - 26%) in “TORNADO-LE” PLS
The following Tab.1 shows the values ratio generating the volume unit of (H2 + CO) mixture per unit of electrical power, which is injected into the plasma under reforming process in the impulse PLS of cylindrical geometry with double pulses mode, and in the “TORNADO-LE”:
\n\t\t\t | \n\t\t\t\tImpulse PLS of cylindrical geometry with double pulses mode\n\t\t\t | \n\t\t\t\n\t\t\t\t"TORNADO-LE"\n\t\t\t | \n\t\t
Single pulse | \n\t\t\t0.027 сm3/Wt | \n\t\t\t\n\t\t |
Double pulses | \n\t\t\t0.0082 сm3/Wt | \n\t\t\t\n\t\t |
Bioethanol 6,5% | \n\t\t\t\n\t\t\t | 0.0024 сm3/Wt | \n\t\t
Bioethanol 13% | \n\t\t\t\n\t\t\t | 0.0079 сm3/Wt | \n\t\t
Bioethanol 26% | \n\t\t\t\n\t\t\t | 0.0615 сm3/Wt | \n\t\t
The volume unit of (H2 + CO) mixture per unit of electrical power in various PLS
The H2 and CO components yield increases with increasing of the ethanol aqueous solution concentration. This concentration has maximum value 26%, and H2 - 26%, CO - 14%. The results of these systems studies show, that the pressure, in region collapse of converging shock waves (with pulse energy > 10 J), exceeds critical (Tab. 2). So, the additional increase chemical activity due to supercritical processes inclusion can be achieved in this situation.
\n\t\t\t\tSolvent\n\t\t\t | \n\t\t\t\n\t\t\t\tMolecular mass\n\t\t\t | \n\t\t\t\n\t\t\t\tCritical temperature, Tcrit\n\t\t\t\t\n\t\t\t | \n\t\t\t\n\t\t\t\tCritical pressure, Pcrit\n\t\t\t\t\n\t\t\t | \n\t\t\t\n\t\t\t\tCritical density, ρcrit\n\t\t\t\t\n\t\t\t | \n\t\t
\n\t\t\t\tg/mol\n\t\t\t | \n\t\t\t\n\t\t\t\tK\n\t\t\t | \n\t\t\t\n\t\t\t\tMPa (bar)\n\t\t\t | \n\t\t\t\n\t\t\t\tg/sm3\n\t\t\t\t\n\t\t\t | \n\t\t|
CO2\n\t\t\t | \n\t\t\t44.01 | \n\t\t\t303.9 | \n\t\t\t7.38 (72.8) | \n\t\t\t0.468 | \n\t\t
H2O | \n\t\t\t18.015 | \n\t\t\t647.096 | \n\t\t\t22.064 (217.755) | \n\t\t\t0.322 | \n\t\t
ethanol | \n\t\t\t46.07 | \n\t\t\t513.9 | \n\t\t\t6.14 (60.6) | \n\t\t\t0.276 | \n\t\t
Critical pаrаmeters of different solvents
The presence of electrolysis phase preceding electrical breakdown of heterophase environment demonstrates that the discharge development in the liquid perform with microbubbles. This result confirms the theory of "bubble" breakdown proposed by Mark Kushner [12].
The formation of convergent acoustic wave after reflection from the ideal solid cylindrical surface was investigated. It is shown that acoustic waves may be effectively focused during these waves passage inside the system.
The research of ethanol reforming in pulse plasma-liquid system has shown that transition from single pulse mode to double pulse mode is accompanied by reduction syn-gase ratio ([H2]/[CO]).
When the working fluid is bioglycerol the K, Na, Ca lines are presented in emission spectra and there is a solid continuous spectrum, which indicates that microparticles are present in the discharge. Its temperature is T = 2800 ± 200 K.
On the base of our results in bioethanol and bioglycerol CO2-reforming by "TORNADO-LE" plasma-liquid system, we can say that:
This process has special features, connected with CO2 retarding role in the conversion components combustion;
In this system there is the possibility of reforming of hydrocarbons with significant viscosity (such as bioglycerol);
All the diagnostic methods, used in the "TORNADO-LE" plasma-liquid system, indicate that there\'re no NOx compounds in the bioethanol and bioglycerol reforming products.
The investigations of bioethanol and bioglycerol in pulse plasma-liquid system have shown:
The main components of the output fuel mixture in this case are: hydrogen, carbon dioxide, and molecular nitrogen, but the carbon dioxide yield is significantly increased in double pulses mode;
The formation of supercritical water in such system and its possible applications for recycling of organic waste and for nanocrystalline particles (in particular, oxide catalysts and other nanocrystalline materials, such as nanotubes) productions needs for additional researches.
The rapid growth of global population as well as industrialization has led to a concomitant increase in environmental pollution. This has very negative effects on natural elements that are vital for life on earth such as air and water. It becomes very crucial therefore to find sustainable ways to mitigate pollution in order to provide a clean and safe environment for humans. Photocatalysis has attracted worldwide interest due to its potential to use solar energy not only to solve environmental problems but also provide a renewable and sustainable energy source. An efficient photocatalyst converts solar energy into chemical energy which can be used for environmental and energy applications such as water treatment, air purification, self-cleaning surfaces, hydrogen production by water cleavage and CO2 conversion to hydrocarbon fuels.
\nResearch in the development of efficient photocatalytic materials has seen significant progress in the last 2 decades with a large number of research papers published every year. Improvements in the performance of photocatalytic materials have been largely correlated with advances in nanotechnology. Of many materials that have been studied for photocatalysis, titanium dioxide (TiO2; titania) has been extensively researched because it possesses may merits such as high photocatalytic activity, excellent physical and chemical stability, low cost, non-corrosive, nontoxicity and high availability [1, 2, 3, 4]. The photocatalytic activity of titania depends on its phase. It exists in three crystalline phases; the anatase, rutile and brookite. The anatase phase is metastable and has a higher photocatalytic activity, while the rutile phase is more chemically stable but less active. Some titania with a mixture of both anatase and rutile phases exhibit higher activities compared to pure anatase and rutile phases [5, 6, 7]. When titania is irradiated with light of sufficient energy, electrons from the valence band are promoted to the conduction band, leaving an electron deficiency or hole, h+, in the valence band and an excess of negative charge in the conduction band. The free electrons in the conduction band are good reducing agents while the resultant holes in the valence band are strong oxidizing agents and can both participate in redox reactions.
\nTitania however suffers from a number of drawbacks that limit its practical applications in photocatalysis. Firstly, the photogenerated electrons and holes coexist in the titania particle and the probability of their recombination is high. This leads to low rates of the desired chemical transformations with respect to the absorbed light energy [8, 9]. The relatively large band gap energy (~ 3.2 eV) requires ultraviolet light for photoactivation, resulting in a very low efficiency in utilizing solar light. UV light accounts for only about 5% of the solar spectrum compared to visible light (45%) [1, 10]. In addition to these, because titania is non-porous and has a polar surface, it exhibits low absorption ability for non-polar organic pollutants [10, 11, 12, 13]. There is also the challenge to recover nano-sized titania particles from treated water in regards to both economic and safety concern [14]. The TiO2 nanoparticles also suffer from aggregation and agglomeration which affect the photoactivity as well as light absorption [15, 16, 17, 18]. Several strategies have been employed in the open literature to overcome these drawbacks. These strategies aim at extending the wavelength of photoactivation of TiO2 into the visible region of the spectrum thereby increasing the utilization of solar energy; preventing the electron/hole pair recombination and thus allowing more charge carriers to successfully diffuse to the surface; increasing the absorption affinity of TiO2 towards organic pollutants as well as preventing the aggregation and agglomeration of the nano-titania particles while easing their recovery from treated water. Several reviews have been published in recent years on the development of strategies to eliminate the limitations of titania photocatalysis [1, 19, 20, 21, 22, 23, 24, 25]. Most of these however focus on pollutant removal from wastewater, water splitting for hydrogen production, CO2 conversion and reaction mechanisms [1, 21, 25, 26, 27, 28, 29, 30, 31]. In this chapter, we review some of the latest publications mainly covering the last 5 years, on strategies that have been researched to overcome the limitations of TiO2 for general photocatalytic applications and the level of success that these strategies have been able to achieve. Based on the current level of research in this field, we also present some perspectives on the future of modified TiO2 photocatalysis.
\nA large number of research works have been published on TiO2 modification to enhance its photocatalytic properties. These modifications have been done in many different ways which include metal and non-metal doping, dye sensitization, surface modification, fabrication of composites with other materials and immobilization and stabilization on support structures. The properties of modified TiO2 are always intrinsically different from the pure TiO2 with regards to light absorption, charge separation, adsorption of organic pollutants, stabilization of the TiO2 particles and ease of separation of TiO2 particles.
\nMetal doping has been extensively used to advance efforts at developing modified TiO2 photocatalysts to operate efficiently under visible light. The photoactivity of metal-doped TiO2 photocatalysts depends to a large extent on the nature of the dopant ion and its nature, its level, the method used in the doping, the type of TiO2 used as well as the reaction for which the catalyst is used and the reaction conditions [32]. The mechanism of the lowering of the band gap energy of TiO2 with metal doping is shown in Figure 1. It is believed that doping TiO2 with metals results in an overlap of the Ti 3d orbitals with the d levels of the metals causing a shift in the absorption spectrum to longer wavelengths which in turn favours the use of visible light to photoactivate the TiO2.
\nBand-gap lowering mechanism of metal-doped TiO2.
Doping of TiO2 nanoparticles with Li, Na, Mg, Fe and Co by high energy ball milling with the metal nitrates was found to widen the TiO2 visible light response range. In the Na-doped sample, Ti existed as both Ti4+ and Ti3+ and the conversion between Ti4+ and Ti3+ was found to prevent the recombination of electrons and (e−) and holes (h+). The metal ion doping promoted crystal phase transformations that generated electrons (e−) and holes (h+) [33]. Mesoporous TiO2 prepared by sol gel technique and doped with different levels of Pt (1–5 wt% nominal loading) resulted in a high surface area TiO2 with an enhanced catalytic performance in photocatalytic water splitting for the Pt-doped samples. The 2.5 wt%Pt-TiO2 had showed the optimum catalytic performance and a reduction in the TiO2 band gap energy from 3.00 to 2.34 eV with an enhanced electron storage capacity, leading to a minimization of the electron-hole recombination rate [34]. Noble metal nanoparticles such as Ag [35], Pt [34], Pd [36], Rh [37] and Au [38] have also been used to modify TiO2 for photocatalysis and have been reported to efficiently hinder electron-hole recombination due to the resulting Schottky barrier at the metal-TiO2 interface. The noble metal nanoparticles act as a mediator in storing and transporting photogenerated electrons from the surface of TiO2 to an acceptor. The photocatalytic activity increases as the charge carriers recombination rate is decreased.
\nIn a recent review by Low et al. [21] the deposition of Au onto TiO2 surface is reported to result in electron transfer from photo-excited Au particles (> 420 nm) to the conduction band of TiO2, which showed a decrease in their absorption band (∼550 nm) and the band was recovered by the addition of electron donors such as Fe2+ and alcohols. Zhang et al. [39] reported that the visible light activity of coupled Au/TiO2 can be ascribed to the electric field enhancement near the metal nanoparticles. Moreover, numerous researchers coupled Au and Ag nanoparticles onto TiO2 surface to use their properties of localized surface plasmonic resonance (LSPR) in photocatalysis [40]. Wang et al. [41] and Hu et al. [42] reported an improved photocatalytic performance due to the Pt nanoparticle which increased the electron transfer rate to the oxidant. It was observed that photocatalytic sacrificial hydrogen generation was influenced by several parameters such as platinum loading (wt%) on TiO2, solution pH, and light (UV, visible and solar) intensities [43]. Moreover, complete discoloration and dye mineralization were achieved using Pt/TiO2 as catalyst; the results were attributed to the higher Pt content of the photocatalyst prepared with the highest deposition time. For Pt-TiO2 catalysts the best discoloration and dye mineralization were obtained over the catalyst prepared by photochemical deposition method and using 120 min of deposition time in the synthesis. These results may be due to the higher Pt content of the photocatalyst prepared with the highest deposition time.
\nHaung et al. [44] prepared Pt/TiO2 nanoparticles from TiO2 prepared at various hydrolysis pH values and found that the phase of TiO2 obtained depended largely on the hydrolysis pH. The anatase/rutile intersection of a Pt/TiO2 sample had a lower recombination rate compared to the anatase phase of Pt/TiO2 due to the longer recombination pathway. Though, the Pt/TiO2 anatase phase showed better degradation efficiency than the Pt/TiO2 anatase/rutile intersection. The decrease in the anatase composition of TiO2, and the decrease in the composition of TiO2 resulted in the degradation rate decrease, suggesting that anatase composition in the Pt/TiO2 system played a crucial role of increasing the photocatalytic degradation of Acid Red 1 dye.
\nLiu et al. [45] prepared the palladium doped TiO2 (Pd-TiO2) photocatalyst using chemical reduction method and tested it the photocatalytic degradation of organic pollutant. It was found that the TiO2 grain size was reduced while the specific surface area increased and the absorption of ultraviolet light also enhanced after using chemical reduction method, however, all these changes had no effect on degradation of organic pollutant. But the degradation was significantly improved due to the deposition of Pd nanoparticles; the Pd/TiO2 organic pollutant degradation was 7.3 times higher compared to TiO2 (P25).
\nRepouse et al. [46] prepared a series of noble metal promoted TiO2 (P25) by wet impregnation and found that the dispersion of the small metal crystallites on TiO2 did not affect the optical band gap of TiO2. The Pt-promoted catalyst exhibited the highest photocatalytic efficiency in the degradation of bisphenol A under solar irradiation. They also found the presence of humic acid to considerably improve the reaction rate of Rh/TiO2 but had a clearly adverse effect with P25 TiO2 photocatalyst. Fluorescence data revealed that humic acid is capable of photosensitizing the Rh/TiO2 catalyst.
\nIndium-doped TiO2 have recently been used for photocatalytic reduction of CO2 [47]. Indium doping resulted in an increase in surface area because of suppression of TiO2 particle growth during the TiO2 synthesis. The light absorption ability of the In-TiO2 was enhanced due to the introduction of the impurity level below the conduction band level of the TiO2. The photocatalytic CO2 reduction activity of the In-TiO2 was about 8 time that of pure TiO2 as a consequence of the high surface area and extended light absorption range.
\nThe doping of TiO2 with transition metals such as Cr [48], Co [48], Fe [48, 49, 50], Ni [48, 51], Mn [48, 52], V [53], Cu [54], Ni [51] and Zn [55], has been studied by different research groups. Numerous studies reported that doping of TiO2 with transition metals improve the photocatalytic activity, attributable to a change in the electronic structure resulting in the absorption region being shifted from UV to visible light. The shift results from charge-transfer transition between the d electrons of the transition metals and the conduct or valence band of TiO2 nanoparticles. Inturi et al. [48] compared the doping of TiO2 nanoparticles with Cr, Fe, V, Mn, Mo, Ce, Co, Cu, Ni, Y and Zr and it was found that Cr, Fe and V showed improved conversions in the visible region while, the incorporation of the other transition metals (Mn, Mo, Ce, Co, Cu, Ni, Y and Zr) exhibited an inhibition effect on the photocatalytic activity. The Cr-doped TiO2 demonstrated a superior catalytic performance and the rate constant was found to be approximately 8–19 times higher than the rest of the metal doped catalysts. It was reported that the reduction peaks in Cr-doped TiO2 shifted to much lower temperatures, due to the increase in the reduction potential of titania and chromium. Therefore, the higher photocatalytic efficiency of Cr/TiO2 in the visible light can be attributed to strong interaction (formation of Cr-O-Ti bonds). Fe-doped TiO2 nanoparticles were used in the visible light degradation of para-nitrophenol and it was found that the Fe-dopant concentration was crucially important in determining the activity of the catalyst. The maximum degradation rate of para-nitrophenol observed was 92% in 5 h when the Fe(3+) molar concentration was 0.05 mol%, without addition of any oxidizing reagents. The excellent photocatalytic activity was as a result of an increase in the threshold wavelength response as well as maximum separation of photogenerated charge carriers [49]. On the other hand, Fe-doped TiO2 evaluated for solar photocatalytic activity for the degradation of humic acid showed a retardation effect for the doped catalysts compared to the bare TiO2 specimens, which could be attributed to surface complexation reactions rather than the reactions taking place in aqueous medium. The faster removal rates attained by using bare TiO2 could be regarded as substrate specific rather than being related to the inefficient visible light activated catalytic performance [50]. Ola et al. [56] reported that the properties of V doped TiO2 were tuned towards visible light because of the substitution of the Ti4+ by V4+ or V5+ ions since the V4+ is centred at 770 nm while the absorption band of V5+ is lower than 570 nm. Moradi et al. [57] obtained high photocatalytic activity of Fe doped TiO2 and studied the effects of Fe3+ doping content on the band gap and size of the nanoparticles. It was found that the increase in the doping content decreased the band gap energy and particle size from 3.3 eV and 13 nm for bare TiO2 to 2.9 eV and 5 nm for Fe10-TiO2, respectively.
\nThe rare earth metals doped TiO2 catalyst also have good electron trapping properties which can result in a stronger absorption edge shift towards longer wavelength, obtaining narrow band gap. Bethanabotla et al. [58] carried out a comprehensive study on the rare earth doping into a TiO2 and found that the rare earth dopants improved the aqueous-phase photodegradation of phenol at low loadings under simulated solar irradiation, with improvements varying by catalyst composition. Differences in defect chemistry on key kinetic steps were given as the explanation for the enhanced performance of the rare earth doped samples compared to pure titania. Reszczyńska et al. [59] prepared a series of Y3+, Pr3+, Er3+ and Eu3+ modified TiO2 nanoparticles photocatalysts and results demonstrate that the incorporation of RE3+ ions into TiO2 nanoparticles resulted in blue shift of absorption edges of TiO2 nanoparticles and could be ascribed to movement of conduction band edge above the first excited state of RE3+. Moreover, incorporated RE3+ ions at the first excited state interact with the electrons of the conduction band of TiO2, resulting in a higher energy transfer from the TiO2 to RE3+ ions. But observed blue shift could be also attributed to decrease in crystallite size of RE3+–TiO2 in comparison to TiO2. The Y3+, Pr3+, Er3+ and Eu3+ modified TiO2 nanoparticles exhibited higher activity under visible light irradiation compared to pure P25 TiO2 and can be excited under visible light in the range from 420 to 450 nm. In a similar work on rare earths (Er, Yb, Ho, Tb, Gd and Pr) titania nanotubes (RE-NTs), [60] the RE3+ species were found to be located at the crystal boundaries rather than inside the TiO2 unit cell and an observed excitation into the TiO2 absorption band with resulting RE3+ emission confirmed energy migration between the TiO2 matrix and RE3+. The presence of the rare earth component was found to reduce recombination of the electrons and holes successfully by catching them and also by promoting their rapid development along the surface of TiO2 nanoparticles. Lanthanide ions doping did not impact the energy gap of TiO2 nanoparticles, however this enhanced the light absorption of catalyst. The surface range of TiO2 nanoparticles generally increases by La3+ particle doping by diminishing the crystallite size and accordingly, the doped TiO2 nanoparticle displayed higher adsorption capacity. Based on theoretical calculations, it was proposed that during the electrochemical process, new Ho-f states and surface vacancies were formed and may reduce the photon excitation energy from the valence to the conduction band under visible light irradiation. The photocatalytic activity under visible light irradiation was attributed not to ·OH but to other forms of reactive oxygen species (O2·−, HO2, H2O2).
\nTiO2 nanoparticles have been comprehensively doped at the O sites with non-metals such as C [61], B [62], I [63], F [64], S [65], and N [66]. Non-metal dopants are reported to be more appropriate for the extension of the photocatalytic activity of TiO2 into visible region compared to metal dopant [67, 68]. This can be ascribed to the impurity states which are near the valence band edge, however, they do not act as charge carriers, and their role as recombination centres might be minimized [53]. As shown in Figure 2, the mixing of the p states of the doped non-metal with the O2p states shifts the valence band edge upward and narrows the band-gap energy of the doped TiO2 photocatalyst. The nitrogen and carbon doped TiO2 nanoparticles has been reported to exhibit greater photocatalytic activity under visible light irradiation compared to other non-metal dopants.
\nBand-gap energy narrowing mechanism for non-metal-doped TiO2.
N-doped TiO2 (N-TiO2) appears to be the most efficient and extensively investigated photocatalyst for non-metal doping. Zeng et al. [69] reported the preparation of a highly active modified N-TiO2 nanoparticle via a novel modular calcination method. The excellent photocatalytic performance of the photocatalyst was ascribed to excellent crystallinity, strong light harvesting and fast separation of photogenerated carriers. Moreover, the enhancement of charge separation was attributed to the formation of paramagnetic [O-Ti4+-N2−-Ti4+-VO] cluster. The surface oxygen vacancy induced by vacuum treatment trapped electron and promoted to generate super oxygen anion radical which was a necessary active species in photocatalytic process. Phongamwong et al. [70] investigated the photocatalytic activity of CO2 reduction under visible light over modified N-TiO2 photocatalyst and they have found that the band gap of N-TiO2 photocatalyst slightly decreases with increasing N content. In addition, the sub-band energies related to the impurity energy level were observed in the N-TiO2 photocatalyst because of the interstitial N species and the sub-band gap energies were found to have decreased from 2.18 eV with 10 wt% N-TiO2 photocatalyst. In contrast, the replacement of O by N is difficult because of the radius of N (17.1 nm) being higher compared to O (14 nm) and the electroneutrality can be maintained by oxygen vacancies, that are provided by replacement of three oxygen vacancies by two nitrogen atom [71]. N-TiO2 photocatalyst reduces the oxygen energy vacancies from 4.2 to 0.6 eV, suggesting that N favors the formation of oxygen vacancies [72].
\nIn contrast, O atoms (14 nm) could be substituted easily by F atoms (13.3 nm) because of their similar ionic radius [73]. Yu et al. [64] reported that the F-doped TiO2 (F-TiO2) is able to absorb visible light due to the high-density states that were evaluated to be below the maxima valence band, although there was no shift in the band edge of TiO2. Samsudin et al. found a synergistic effect between fluorine and hydrogen in hydrogenated F-doped TiO2 which enabled light absorption in UV, visible and infrared light illumination with enhanced electrons and holes separation. Surface vacancies and Ti3+ centres of the hydrogenated F-doped catalyst coupled with enhanced surface hydrophilicity facilitated the production of surface-bound and free hydroxyl radicals. Species present on the surface of the catalyst triggered the formation of new Ti3+ occupied states under the conduction band of the hydrogenated F-doped TiO2, thus narrowing the band gap energy [73]. Enhanced photocatalytic performance of N-doped TiO2 over pure TiO2 has also been ascribed to efficient separation of electron-hole pairs as well as an increased creation of surface radicals such as hydroxyl The band gap can also be narrowed by doping TiO2 with S, since replacement of S into TiO2 can be performed easily due to larger radius of S atoms (18 nm) compared to O atoms (14 nm). S incorporation in TiO2 has been reported to change the lattice spacing of the TiO2 with a reduction in the band gap width from 3.2 to 1.7 eV allowing for higher photocatalytic activity [74]. N, S and C co-doped TiO2 samples photocatalytic reduction of Cr(IV) showed that the co-doping and calcination played an important role in the microstructure and photocatalytic activity of the catalysts. The co-doped samples calcined at 500°C showed the highest activities ascribed to the synergistic effect in enhancing crystallization of anatase and (N, S and C) co-doping. The carbon doped TiO2 (C-TiO2) is reported to be more active than N-TiO2, therefore, C-TiO2 has received special attention [75]. Noorimotlagh et al. [76] investigated the photocatalytic removal of nonylphenol (NP) compound using visible light active C-TiO2 with anatase/rutile. It was found that the doping of C into TiO2 lattice may enhance the visible light utilization and affect the structural properties of the as-synthesized photocatalysts. Moreover, it was reported that after C doping and changing the calcination temperature, the band gap was narrowed from 3.17 to 2.72 eV and from 2.72 to 2.66 eV, respectively. Ji et al. [61] reported the preparation of C-TiO2 with a diameter of around 200 nm and the tube wall was composed of anatase TiO2, amorphous carbon, crystalline carbon and carbon element doping into the lattice of TiO2. The C-TiO2 nanotubes exhibited much better performance in photocatalytic activity than bare TiO2 under UV and visible light. The obtained results were ascribed to the C doping, which narrowed the band gap energy of TiO2, extended the visible light adsorption toward longer wavelength and hindered charge recombination.
\nAlthough single metal doped and non-metal doped TiO2 have exhibited excellent performance in decreasing the electrons and holes recombination, but they suffer from thermal stability and losing a number of dopants during catalyst preparation process [77]. Therefore, co-doping of two kinds of atoms into TiO2 has recently attracted much interest [78]. The electronic structure of TiO2 can be altered by co-doping on TiO2 by formation of new doping levels inside its band gap. Abdullah et al. [77] reported that the doping levels situated within the band gap of TiO2 can either accept photogenerated electrons from TiO2 valence band or absorb photons with longer wavelengths. Therefore, suggesting that the TiO2 absorption range can be expanded.
\nZang et al. [79] evaluated the photocatalytic degradation of atrazine under UV and visible light irradiation by N,F-codoped TiO2 nanowires and nanoparticles in aqueous phase. It was found that photocatalytic degradation of atrazine was higher in the presence of N,F-codoped TiO2 nanowires than that of N,F-codoped TiO2 nanoparticles. The higher photocatalytic performance in the presence of N,F-codoped TiO2 nanowires was attributed to the higher charge carrier mobility and lower carrier recombination rate. Moreover, the speed of electron diffusion across nanoparticle intersections is several orders of magnitude smaller compared to that of nanowire because of frequent electron trapping at the intersections of nanoparticles and increasing the recombination of separated charges before they reach the TiO2 nanoparticles surface. Park et al. [80] showed the best performance for novel Cu/N-doped TiO2 photoelectrodes for dye-sensitized solar cells. It was found that the Cu/N-doped TiO2 nanoparticles provided higher surface area, active charge transfer and decreased charge recombination. Moreover, the addition of suitable content of Cu- to N-doped TiO2 electrode effectively inhibited the growth of TiO2 nanoparticles and improved the optical response of the photoelectrode under visible light irradiation. Chatzitakis et al. [81] studied the photoelectrochemical properties of C, N, F codoped TiO2 nanotubes. It was found that increasing surface area is not followed by increase in the photoconversion efficiency, but rather that an optimal balance between electroactive surface area and charge carrier concentration occurs.
\nZhao et al. [82] investigated the photocatalytic H2 evolution performance of Ir-C-N tridoped TiO2 under UV-visible light irradiation. The photocatalytic activity of TiO2 nanoparticles was reported to be improved by Ir-C-N tridoped TiO2 under UV-visible light, due the synergistic effect between Ir, C and N on the electron structure of TiO2. It was found that Ir existed as Ir4+ by substituting Ti in the lattice of TiO2 nanoparticles, whereas the C and N were also incorporated into the surface of TiO2 nanoparticles in interstitial mode. The absorption of TiO2 nanoparticles was expanded into the visible light region and the band gap was narrowed to ~3.0 eV, resulting in improved photocatalytic H2 evolution under UV-visible light irradiation. Tan et al. [83] investigated the photocatalytic degradation of methylene blue by W–Bi–S-tridoped TiO2 nanoparticles. It was found that the absorption edge of TiO2 was expanded into visible-light region after doping with W, Bi and S and the catalytst showed the best photocatalytic activity, than that of TiO2, S-TiO2, W–S–TiO2 and Bi–S–TiO2. This might be attributed to the synergistic effect of W, Bi and S.
\nAmongst the various strategies that have been used to enhance TiO2 photocatalytic activity, improvement of morphology, crystal structure and surface area have also been considered important and widely investigated approach to achieve better photocatalytic performance. The nanotitania crystallinity can simply be enhanced by optimizing the annealing temperature. However, the stability of the structure and geometries have to be considered when annealing [84]. For the nanotitania morphology and surface area, various ordered structures have been studied. TiO2 nanotubes [85, 86], nanowires [79], nanospheres [87], etc. Tang et al. fabricated monodisperse mesoporous anatase TiO2 nanospheres using a template material and found the resulting catalysts to show high photocatalytic degradation efficiency and selectivity towards different target dye molecules and could be readily separated from a slurry system after photocatalytic reaction [87]. Anodic TiO2 nanotubes have been reported to allow a high control over the separation of photogenerated charge carriers in photocatalytic reactions. The nanotube array has as key advantage the fact that nanotube modifications can be embedded site specifically into the tube wall or at defined locations along the tube wall. This allows for engineering of reaction sites giving rise to enhanced photocatalytic efficiencies and selectivities [88].
\nThe design and preparation of graphene-based composites containing metal oxides and metal nanoparticles have attracted attention for photocatalytic performances. For example, Tan et al. [89] prepared a novel graphene oxide-doped-oxygen-rich TiO2 (GO–OTiO2) hybrid heterostructure and evaluated its activity for photoreduction of CO2 under the irradiation of low-power energy-saving daylight bulbs. It was found that the photostability of O2–TiO2 was significantly improved by the addition of GO, at which the resulting hybrid composite retained a high reactivity. The photoactivity attained was about 1.6 and 14.0 folds higher than that of bare O2–TiO2 and the commercial Degussa P25, respectively. This high photocatalytic performance of GO–OTiO2 was attributed to the synergistic effect of the visible-light-responsiveness of O2–TiO2 and an enhanced separation and transfer of photogenerated charge carriers at the intimate interface of GO–OTiO2 heterojunctions. This study is reported to have opened up new possibilities in the development of novel, next generation heterojunction photocatalysts for energy and environmental related applications. Lin et al. [90] also investigated photoreduction of CO2 with H2O vapor in the gas-phase under the irradiation of a Xe lamp using TiO2/nitrogen (N) doped reduced graphene oxide (TiO2/NrGO) nanocomposites. They found that the quantity and configuration of N dopant in the TiO2/NrGO nanocomposites strongly influenced the photocatalytic efficiency, and the highest catalytic activity was observed for TiO2/NrGO nanocomposites with the highest N doping content. Moreover, modified TiO2/rGO demonstrated a synergistic effect, enhancing CO2 adsorption on the catalyst surface and promoting photogenerated electron transfer that resulted in a higher CO2 photoreduction rate of TiO2/NrGO. Qu et al. [91] prepared the graphene quantum dots (GQDs) with high quantum yield (about 23.6% at an excitation wavelength of 320 nm) and GQDs/TiO2 nanotubes (GQDs/TiO2 nanoparticles) nanocomposites and the photocatalytic activity was tested towards the degradation of methyl orange. It was found that the GQDs deposited on TiO2 nanoparticles can expand the visible light absorption of TiO2 nanoparticles and enhance the activity on photocatalytic degradation of methyl orange under UV-vis light irradiation (ʎ = 380–780 nm). Furthermore, the photocatalytic activity of GQDs/TiO2 nanoparticles was approximately 2.7 times as higher than that of bare TiO2 nanoparticles. Tian et al. [92] reported the preparation of N, S co-doped graphene quantum dots (N, S-GQDs)-reduced graphene oxide- (rGO)-TiO2 nanotubes (TiO2NT) nanocomposites for photodegradation of methyl orange under visible light irradiation. It was found that the S-GQDs+rGO + TiO2 nanocomposites simultaneously showed an extended photoresponse range, improved charge separation and transportation properties. Moreover, the apparent rate constant of N, S-GQDs+rGO + TiO2NT is 1.8 and 16.3 times higher compared to rGO + TiO2NT and pure TiO2NT, respectively. Suggesting that GQDs can improve the utilization of solar light for energy conversion and environmental therapy.
\nAnother drawback of TiO2 nanoparticles mentioned above is the formation of uniform suspension in water which makes its recovery difficult, therefore hindering the application of photocatalytic in an industrial scale. As a result, many studies have attempted the modification of TiO2 nanoparticles on support materials such as clays [93, 94] quartz [95], stainless steel [96], etc. Clays have been reported to be a significant support material for TiO2 nanoparticles because of their layered morphology, chemical as well as mechanical stability, cation exchange capacity, non-toxic nature, low cost and availability. Therefore, TiO2/clay nanocomposites have attracted much attention for application in both water and air purification and have been prepared by numerous researchers. Belver et al. [97] investigated the removal of atrazine under solar light using a novel W-TiO2/clay photocatalysts. It was found that the photocatalytic activity of W-TiO2/clay catalyst exhibited higher photocatalytic performance than that of an un-doped TiO2/clay, which was explained by the presence of W ions in the TiO2 nanostructure. The substitution of Ti ions with W resulted in the increase of its crystal size and the distortion of its lattice and moderately narrower band gap of photocatalysts. Mishra et al. [98] reported the preparation of TiO2/clay nanocomposites for photocatalytic degradation of VOC and dye. They found that the photocatalytic performance of TiO2/clay nanocomposites is highly dependent on the clay texture (as 2:1 clays show highest activity than 1:1) apart from their surface area and porosity. Moreover, the reactions involving TiO2/Clay photocatalyst were fast with rate constant of 0.02886 and 0.04600 min−1 for dye and VOC respectively than the other nanocomposites.
\nIn this chapter, we have given an overview of the development of modified TiO2 catalysts and its future prospects from a scientific point of view. We note that the field has experienced major advances in the last 5 years especially in the area of modifying TiO2 with carbon nanomaterials. Based on the literature we have covered here, we believe that there is still quite a lot that can be achieved in improving the performance of TiO2 catalysts for photocatalytic applications.
\nThere are no conflicts of interest to declare.
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