Summary of gasification simulation of various materials using Aspen Plus from literature.
In this era of plastics dominated world, it remains a fact that there exists an ever-increasing margin between the volume of waste plastics generated and the volume recycled . Of the total plastic waste, recyclable thermoplastics like polyethylene, polystyrene, polypropylene and PVC account for nearly 78% of the total and the rest is composed of the non-recyclable thermosets like epoxy resins and polyurethane . Typically, plastics waste management is practiced according to the following hierarchical order: Reduction, Reuse, Recycling, and finally energy recovery. Although reuse of plastics seems to be best option to reduce plastic wastes, it becomes unsuitable beyond certain cycles due to the degradation of plastic. Mechanical recycling of plastics involves significant costs related to collection and segregation, and is not recommended for food and pharmaceutical industries. While chemical recycling focuses on converting waste plastics into other gaseous or liquid chemicals that act as a feedstock for many petrochemical processes, energy recovery utilizes the stored calorific value of the plastics to generate heat energy to be used in various plant operations. Moreover, since plastic wastes always consist of a mixture of various polymeric substances, chemical recycling and energy recovery seems to be best possible solution, both in terms of economic and technological considerations.
One of the major processes of chemical recycling involves thermal treatment of the waste plastics. The inevitable shift in world’s energy paradigm from a carbon based to hydrogen based economy has revolutionized the capabilities of thermal treatment processes, viz. combustion, gasification and pyrolysis, in particular on the latter two techniques. In fact, recent technical investigations on the novel municipal solid waste (MSW) management methods reveal that a combined gasification and pyrolysis technique is more energy efficient and environmentally friendly than other processes .
In general the process of gasification for energy extraction from solid carbon source involves three simultaneous or competing reactions namely combustion, pyrolysis and gasification. The partial combustion of solid fuel creates an oxygen devoid, high temperature condition within the reactor which promotes the pyrolysis reaction, breaking the fuel into products that are a mixture of char and volatiles containing small and long chain hydrocarbons. The presence of gasifying agent (steam) drives the water shift reaction converting the carbon sources in to a mixture of valuable chemicals, tar, fuel gases and some residual particulate matter. The products undergo various downstream operations in order to separate and purify the valuable gaseous products that are later utilized for energy generation. This auto thermal feature makes the gasification process an economically viable and efficient technique for recovery of energy from waste plastics.
Gasification in commercial scale is practiced based on batch, semi batch and continuous modes of operation depending upon the processing capacity of the plant. Typically a plant processing large throughput utilizes fluidized beds due to the advantages such as enhanced gas-solid contact, excellent mixing characteristics , operating flexibility , and ease of solids handling  that lead to a better overall gasification efficiency. Fluid beds are preferred as it offers high heat and mass transfer rate and a constant reaction temperature which results in a uniform spectrum of product in a short residence time. It is important to keep the good fluidization characteristics of the bed, since introduction of material with different properties than the original components of the bed affect the quality of fluidization. Introduction of plastic material in fluidized beds demand additional attention due to its softening nature and possibility of blocking the feeding line. As soon as the plastic enters the hot reaction zone, it thermally gets cracked and undergoes a continuous structural change until it is eliminated from the bed. The sequence of interaction between the inert particle in the fluidized bed and the plastic material has been narrated by Mastellone et al., .
Gas-solid fluidization is the operation by which a bed of solid particles is led into a fluid-like state through suspension in a gas. Large scale gasifiers employ one of the two types of fluidized bed configurations: bubbling fluidized bed and circulating fluidized bed. A bubbling fluidized bed (BFB) consists of fine, inert particles of sand or alumina, which are selected based on their suitability of physical properties such as size, density and thermal characteristics. The fluidizing medium, typically a combination of air/nitrogen and steam, is introduced from the bottom of the reactor at a specified flow rate so as to maintain the bed in a fluidization condition. The dimension of the reactor section between the bed and the freeboard is designed to progressively expand so as to reduce the superficial gas velocity which prevents solid entrainment, and to act as a disengaging zone. A cyclone is provided at the end of the fluidized bed either to return fines to the bed or to remove fines from the system. The plastic waste is introduced into the fluidized bed at a specified location, either
One of the main disadvantages of fluidized bed is the formation of large bubbles at higher gas velocities that bypass the bed reducing transfer rates significantly. If the gas flow of a bubbling fluidized bed is increased, the gas bubbles become larger forming large voids in the bed entraining substantial amounts of solids. The bubbles basically disappear in a circulating fluidized bed (CFB) and CFB the solids are separated from the gas using a cyclone and returned back to the bed forming a solids circulation loop. A CFB can be differentiated from a BFB in that there is no distinct separation between the dense solids zone and the dilute solids zone. The residence time of the solids in the circulating fluid bed is determined by the solids circulation rate, attrition of the solids and the collection efficiency of the solids in the cyclones. The advantages of the circulating fluidized bed gasifiers are that they are suitable for rapid reactions resulting in high conversion The disadvantage being, i) temperature gradients in the direction of the solid flow, ii) limitation on the size of fuel particles iii) high velocities resulting in equipment erosion. Although there are many different types of fluidized beds available for gasification and combustion, bubbling fluidized type is the most preferred type whenever steam is used as a gasifying medium . The advantages of steam gasification have been well addressed in the literature .
A wide variety of plastics are in use depending upon the type of application, of which the most widely utilized are polyethylene (PE), Polypropylene (PP), Polyvinyl chloride (PVC), Polystyrene (PS) and Polyethylene terephthalate (PET). Each type differs in physical and chemical properties, and so do their applications. In general, the combustion of most of the plastics is considered safe with the exception of PVC that generates dioxins due to the presence of chlorine compound in its structure. In contrast with combustion, pyrolysis and gasification are endothermic process which require substantial amount of energy to promote the reactions. The pyrolysis process generally produces gas, liquid and solid products, the proportions of which depends on the operating conditions, while the gasification is predominantly reactions involving carbon or carbon-based species and steam, producing syngas (CO and H2) and minor higher molecular weight hydrocarbons .
Cracking of PE either into its constituent monomer or other low molecular weight hydrocarbons has become a vital process due to the increased amounts of polyethylene wastes in the present world. Pyrolysis and/or gasification of PE serve as an appropriate tool for the recovery of energy and for waste plastic disposal simultaneously. Compared with other alternative feedstock like biomass and coal, PE possesses relatively higher heating value, and is much cleaner in terms of fuel quality attributing to lesser fuel pre-processing costs. Pyrolysis or gasification of PE results in a product stream rich in hydrogen and minimal CO or CO2 content as compared to cellulose based wastes that yields relatively higher carbon monoxide and lower hydrogen product composition mainly due to the presence of oxygen in cellulose based feedstock.
Irrespective of the type of reactor and type of waste being handled, the key operating parameters that play a vital role in the gasification process are the equivalence ratio, reactor temperature, steam to fuel ratio, gasifying medium and residence time. In order to exert better reliability of the system, the operating variables have to be optimized and controlled with significant accuracy. The cheapest and most effective technique to qualitatively understand the effect of each operating variable and to identify possible optimal conditions is through process simulation. Such attempts to develop simulation models for process optimization has been reported in open literature of fuel sources such as, tyre , coal [10-13], and biomass [8, 14-16] using various computer simulation packages. However, the utility of any process simulation tool has not been well explored or recorded in the literature for modeling plastics gasification.
This chapter discusses recent work by the authors on Aspen Plus based process model to analyze the performance of a plastics gasification process under equilibrium conditions. The primary goal of this work is to successfully test and demonstrate the applicability of Aspen Plus to simulate the gasification process for one of the most abundantly used plastic, polyethylene (PE). This study will serve some preliminary qualitative and quantitative information on the overall behavior of the gasification process including the sensitivity of process parameters.
2. Model development
2.1. Modeling the gasification process
The gasification process models available in literature can be generally classified under steady state or quasi-steady state or transient state models. The steady state models do not consider the time derivatives and are further classified as kinetics
The model used in this work to investigate the simulation of PE gasification in fluidized bed reactor is based on the model previously developed by Mitta et al.  for simulating tyre gasification. The
|Temperature (°C)||700-900||Higher temperature, lower ER and higher steam-to-fuel ratio favors hydrogen and CO production|
Boudouard and methanation reactions were not considered
|Steam to fuel ratio||0-4|
|Tyre||Equilibrium||Temperature (°C)||750 -1100||Higher temperature, higher fuel/air ratio and lower steam/fuel ratio favors hydrogen and CO production|
All components listed in gasification reactions, along with H2S, are considered as possible products
|Fuel to air ratio||0.2-0.8|
|Steam to fuel ratio||1.25-5|
|Biomass||Restricted Equilibrium||Temperature (°C) (achieved by changing ER between 0.29 -0.45)||674-1195||Air preheating effective at ER’s less than 0.35|
Without air preheating, optimum conditions for ER is 0.34 and gasification temperature between 837 to 874 °C
Only Reactions (1-8) along with reactions for the formation of H2S and NH3 were considered for Gibbs free energy minimization
|Air Preheating Temperature (°C)||25-825|
The following assumptions are made in the current study for developing the process model.
All the chemical reactions were assumed to have reached equilibrium within the gasifier.
Only methane, hydrogen, carbon monoxide, carbon dioxide, oxygen, nitrogen, H2S, and water were considered to be present in the product stream.
The primary components of char are only carbon and ash.
The entire gasification process was modeled using Aspen’s
2.1.1. Fuel pre-processing
Figure 1 illustrates the process flow sheet of the
At first, the fuel stream was first introduced into a drying unit “DRIER”, which was modeled in Aspen Plus using an RSTOIC module. A temperature of 110 ºC and a pressure of 1 atm were selected as drier operating conditions. The stream leaving the drier, labeled “DRIED” contains the dried PE in solid phase and the removed moisture in vapor phase. This stream was fed to a separation unit “SEPARATOR” that splits the feed stream into product streams, labeled as “DRYPE” and “MOISTURE”.
2.1.2. Volatiles and char gasification
In a typical gasification process, the fuel is first pyrolyzed by applying external heat where it breaks into simpler constituent components. These volatile components, along with char are then combusted, and the heat liberated from the combustion reactions would be used up by the subsequent endothermic gasification reactions. In the Aspen plus model, the dried portion of the fuel “DRYPE” exiting from the “DRIER” enters a pyrolyzer “PYROL” modeled as a RYIELD block in Aspen Plus. Based on the ultimate analysis of PE shown in Table II, the product yield distribution was calculated in the RYIELD module using Aspen Plus built-in calculator. An operating temperature of 500 ºC and a pressure of 1 atm were chosen in order to set the exiting stream “VOLATILE” to a pre-heated temperature of 500 ºC.
|Fuel feed rate||constant||6 kg/h|
|Air flow rate||variable||5 – 30 kg/h|
|Steam flow rate||variable||0.3 – 30 kg/h|
|Air temperature||constant||773 K|
|Steam temperature||constant||773 K|
|Pyrolyzer temperature||constant||773 K|
|Drier temperature||constant||383 K|
|Heat of Reaction (kJ/mol)|
T =1000 K, P = Po
|1||C + ½ O2 ↔ CO||-112||Reactions with oxygen|
|2||CO + ½ O2 ↔ CO2||-283|
|3||H2 + ½ O2 ↔ H2O||-248|
|4||C + H2O ↔ CO + H2||136||Reactions with water|
|5||CO + H2O ↔ CO2 + H2||-35|
|6||CH4 + H2O ↔ CO + 3H2||206|
|7||C + CO2 ↔ 2CO||171||Boudouard reaction|
|8||C + 2H2 ↔ CH4||- 74.8||Methanation reactions|
|9||CO + 3H2 ↔ CH4 + H2O||-225|
|10||CO2 + 4H2 ↔ CH4 + 2H2O||-190|
The volatiles stream, along with char was then passed to a gasifying unit “GASIFIER” that was modeled as a RGIBBS module. As it can be noticed in the model, the combustion and gasification reactions are allowed to take place within the “RGIBBS” module itself. The RGIBBS module calculates the equilibrium composition of the system using Gibbs free energy minimization technique. It provides an option to either consider all the components present in the system as equilibrium products or restrict the components based on some specific reactions or restrict it based on a temperature approach. In this study, all components from the gasification reactions, listed in Table IV, along with H2S were included as possible fluid phase or solids products in the RGIBBS module. The gasifying mediums, air and steam, are preheated and mixed before it is sent to the gasifier. The outlet stream labeled as “PRODUCTS” contains product gases resulting from the gasification process while the “ASH” stream contains any residual solids.
The flow rate of fuel stream was held constant at 6 kg/h for all simulations. The two key parameters that influence the reactor temperature and the product distribution are equivalence ratio and the steam-fuel ratio, and hence were the only variables considered in the simulation. Equivalence ratio can be defined as the ratio of mass of oxygen/air supplied to the mass of oxygen/air necessary for complete combustion of all the carbon and hydrogen present in the feed to carbon dioxide and water respectively.
2.2. Model validation
The base case model for the gasification process was developed using Aspen plus built in modules based on the simulations popularly adopted in literature. In order to validate the appropriateness of the present model, simulations have been performed for gasification of tyre and the results were compared with the work due to Mitta et al. . The ultimate and proximate analysis data used for tyre simulation in this study has been listed in Table II. However since the simulation parameters were not fully detailed by the authors, the parameters utilized in the present simulation is not the same as reported by Mittal et al. Therefore, only a qualitative comparison of the effect of parameters on the product distribution was considered for comparison purposes. Results showed good agreement in terms of the trends of the composition
In this work, a similar kind of study was performed to investigate the performance characteristics of the PE gasification process. In the case of isothermal gasification studies, it is challenging to include the temperature variation effects resulting from the entering steam flow, and exclusion of which results in significant deviation in the simulation results . Hence, in this work, an adiabatic type of gasification reactor was modeled to investigate the effects of two key parameters, namely the equivalence ratio and steam-to-fuel ratio. The response variables include the gas composition, Carbon monoxide efficiency, hydrogen efficiency, and combined CO and hydrogen efficiency.
The carbon monoxide efficiency measures the extent of conversion of carbon present in the fuel to carbon monoxide. The definition of hydrogen efficiency and the combined efficiency follows the same. Van den Bergh  has reported expressions to calculate the CO, H2, and combined CO and H2 efficiencies. A similar definition was introduced in this work to estimate carbon dioxide efficiency as shown below.
where, and represents the volume fraction of CO and CO2 in the product gas respectively, is the rate of carbon feeding [moles of carbon/min],
3. Results and discussion
3.1. Effect of steam-to-PE ratio
The effect of steam-to-PE mass ratio on PE gasification process was investigated in the range of 0.05 to 5 (corresponding to a mole ratio of 0.04 to 3.9) with a constant PE feed rate of 6 kg/h and an equivalence ratio of 0.15 (air flow rate of 15 kg/h). It can be expected that at low concentrations of water, oxidation reactions
Figure 2 illustrates the variation of product molar composition and the equilibrium reactor temperature as a function of steam-to-PE mass ratio. The simulation
Figure 3 shows the effect of the steam-to-PE ratio on the fractional efficiency of CO, CO2 and H2. It is evident that at around a steam-to-PE ratio of 0.4, the production of CO and hydrogen peaks while that of carbon dioxide is at a minimum. This is a favorable condition for any waste gasification process where it is desired to minimize as much as carbon dioxide as possible. Hence, it can be concurred that the favorable steam-to-PE mass ratio for the gasification process should be between 0.4 and 0.6, where the combined as well as the individual compositions of CO and H2 are at a maximum. Furthermore, the cold gas efficiency (CGE) of the process seems to be affected only at lower steam-to-PE ratio. The predicted CGE values are much higher than those obtained in typical waste gasification process which is about 60%. It can be expected that under equilibrium conditions, as considered in this study, the gas yield is significantly higher than real process which directly contributes to increased efficiency.
3.2. Effect of equivalence ratio
The effect of equivalence ratio on the overall gasification efficiency was studied at two different steam-to-PE ratios. Typically, a commercial biomass gasifier is operated at an ER value of 0.25 in order to maintain auto thermal conditions (van den Bergh, 2005). Hence, a range of 0.05 to 0.3 was selected for this study in order to determine the optimum ER for PE gasification process. The cases for the two different steam-to-PE ratios have been presented and discussed separately below.
The oxidation reactions of carbon, CO and hydrogen, depicted by Reactions (1-3) are spontaneous and exothermic, resulting in release of significant amount of heat energy. It can be expected through Reaction (1) that at low values of ER (low values of stoichiometric air), only incomplete combustion of carbon would take place leading to the formation of CO with release of heat. Therefore, for the range of ER considered in this study, only Reactions (1) and (3) are the possible oxidation reactions, and thus any heat released during the combustion process will be directly attributed to these two reactions.
In general, at any fixed steam-to-PE ratio, the other parameters that drive the gasification process would be the ER and consequently the heat released from the combustion reactions. The intensity of the heat released controls the temperature, which in turn affects the directional shift in equilibrium of the gasification reactions. For example, the endothermic reactions (4, 6, and 7) would tend to shift in the forward direction with an increase in temperature and
At low ER and low steam content, Reactions (4, 5 and 7) would be possibly controlled by the temperature and the partial pressure of steam. At such conditions, it could be expected that Reaction (5) would not be driven forward resulting in lower carbon dioxide formation. Furthermore, at low ER values, reactions with water would significantly compete with the oxidation reactions, thus limiting the resulting equilibrium temperature. At high ER and low steam content, this effect would be compounded such that temperature would be the primary variable that would determine the direction of the gasification reactions. In addition, at higher ER the composition trend of CO could be expected to fall down due to the subsequent combustion and methanation reactions of CO.
Figure 4 illustrates the variation of product gas composition and temperature as a function of various equivalence ratios. Between ER values of 0.05 and 0.2, reactor temperature, CO content, and hydrogen content increases steadily while the composition of methane decreases very sharply. In addition, the composition of carbon dioxide shows a steady decrease whereas the molar composition of water remains a constant. At ER values higher than 0.2, it can be observed that the temperature increases very sharply along with a steady decrease of hydrogen and carbon monoxide. It can also be noticed that beyond this point, only hydrogen, CO, and water are the major components of the product stream. The low values of carbon dioxide predicted throughout the range can be explained by the fact that at such low ER and steam-to-PE ratios considered in this study, neither complete oxidation nor steam gasification of carbonaceous components, depicted by reactions (2) and (5) respectively, proceeds at any significant rate. The sharp increase in the temperature beyond ER = 0.2 is due to the domination of the exothermic combustion reactions over others. The simulation results are very much in agreement with the theoretical expectations discussed earlier in this section.
Figure 5 illustrates the variation of the fractional efficiencies with the equivalence ratios. It is clear that the efficiency of the conversion proceeds rapidly at lower ER’s and reaches a maximum at ER of 0.2 and at a fixed steam-to-PE ratio of 0.6. The effect of ER on CGE is not significant at lower values since the composition of CO, hydrogen and methane that directly contribute to the heating value of the product gas increases until ER = 0.2. Beyond this point, since the yield of the above products decreases, CGE follows a decreasing trend and records a value of about 75% at an ER value of 0.3.
An additional study of the effect of ER on the gasification process at a higher steam-to-PE ratio was included to provide better and comprehensive understanding of the sensitivity of equivalence ratio. In this case, the gasification reactions would not only be driven by the heat released by the preceding combustion reactions, but also by the partial pressure of steam. At a higher steam-to-PE ratio, it could be expected that Reaction (4) would significantly compete with Reaction (1) to consume the carbon present in the feed. Hence, the absolute value of the equilibrium temperature would be lower when compared to the previous case, steam-to-PE ratio of 0.6. Although high ER values would restrict the forward shift of the exothermic Reaction (5), the presence of higher steam content would favor the equilibrium to shift in the forward direction resulting in higher net carbon dioxide content.
Referring to Figures 4 and 6, it is evident that the trends of composition and temperature follow the same as case 1, but with different absolute values. It should be noted that the simulations predicted a temperature of about 800 K at an ER of 0.1 for case 2 compared to a value of ca. 850 K for case 1. It can also be observed that the composition of carbon dioxide was slightly higher and that of carbon monoxide was significantly lower than the results reported earlier in Case 1.
It can also be noticed from Figures 5 and 7 that the absolute maximum value of the combined CO and H2 efficiency is significantly different among the two cases, which are predicted as 40% for case 1 and 7% for case 2. The composition of carbon dioxide in the product gases is very negligible at lower steam content, while it reaches about 4% for the case of higher steam content. Nevertheless, in both the cases, the maximum fractional efficiency of all the components occurs at an ER value of ca. 0.2. Furthermore, as discussed earlier in section 3.1, the effect of steam-to-PE ratio ion CGE is remarkable only until 0.6. Thus, the trend of CGE in Figure 7 for the case of higher steam-to-PE ratio resembles the same as that of Figure 5.
Hence, it can be concluded that an ER value of 0.2 and steam-to-PE ratio of 0.4 to 0.6 would yield a product stream containing 35% hydrogen, 25% CO, and negligible CO2 at a temperature of 1000 K. These values seem acceptable for all practical purposes and are very much in agreement with the literature data, where a value steam-to-fuel value of 0.42 and an ER value of 0.15 were reported as the optimum parameters for co-gasification of wood and polyethylene .
The gasification process of waste polyethylene was successfully modeled using a combination of various unit operation modules available in Aspen Plus simulation package. The model used in this work to investigate the simulation of PE gasification in fluidized bed reactor is based on the model previously reported in literature for simulating waste tyre gasification. The equilibrium model developed in this study enables one to predict the behavior of PE gasification process under various operating conditions. Moreover, the results obtained are easy to interpret and thus could be directly corroborated with actual plant data.
Although temperature plays a vital role in controlling the conversion and product composition, it has been treated as a
Optimum steam-to-PE ratio was determined to be between 0.4 and 0.6 for low temperature applications. Under this condition, the yield of syngas and cold gas efficiency reaches a maximum.
Product gas temperatures as high as 1273 K could be attained at higher steam-to-PE ratio at the expense of decrease in calorific value
Sensitivity analysis on ER proposes an optimum value of about 0.2. Both CGE and syngas efficiency reaches a maximum at this point.
Due to the lack of detailed experimental data on waste PE gasification for various process conditions, the predicted data could not be validated. Although the results from this work heavily depend on the assumption made, i.e. thermodynamic equilibrium, significant qualitative results were deduced that would help to establish a sound reference for any detailed process optimization studies. Furthermore, this model can be used to estimate the final gas composition and other parameters, including gas yield and temperature for other solid waste fuels and mixtures. Upon including the hydrodynamics and gasification kinetics, this model could be used to evaluate the performance and behavior of many types of gasifiers under different process conditions.
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