Differential diagnosis of allergic and local allergic rhinitis.
\\n\\n
Dr. Pletser’s experience includes 30 years of working with the European Space Agency as a Senior Physicist/Engineer and coordinating their parabolic flight campaigns, and he is the Guinness World Record holder for the most number of aircraft flown (12) in parabolas, personally logging more than 7,300 parabolas.
\\n\\nSeeing the 5,000th book published makes us at the same time proud, happy, humble, and grateful. This is a great opportunity to stop and celebrate what we have done so far, but is also an opportunity to engage even more, grow, and succeed. It wouldn't be possible to get here without the synergy of team members’ hard work and authors and editors who devote time and their expertise into Open Access book publishing with us.
\\n\\nOver these years, we have gone from pioneering the scientific Open Access book publishing field to being the world’s largest Open Access book publisher. Nonetheless, our vision has remained the same: to meet the challenges of making relevant knowledge available to the worldwide community under the Open Access model.
\\n\\nWe are excited about the present, and we look forward to sharing many more successes in the future.
\\n\\nThank you all for being part of the journey. 5,000 times thank you!
\\n\\nNow with 5,000 titles available Open Access, which one will you read next?
\\n\\nRead, share and download for free: https://www.intechopen.com/books
\\n\\n\\n\\n
\\n"}]',published:!0,mainMedia:null},components:[{type:"htmlEditorComponent",content:'
Preparation of Space Experiments edited by international leading expert Dr. Vladimir Pletser, Director of Space Training Operations at Blue Abyss is the 5,000th Open Access book published by IntechOpen and our milestone publication!
\n\n"This book presents some of the current trends in space microgravity research. The eleven chapters introduce various facets of space research in physical sciences, human physiology and technology developed using the microgravity environment not only to improve our fundamental understanding in these domains but also to adapt this new knowledge for application on earth." says the editor. Listen what else Dr. Pletser has to say...
\n\n\n\nDr. Pletser’s experience includes 30 years of working with the European Space Agency as a Senior Physicist/Engineer and coordinating their parabolic flight campaigns, and he is the Guinness World Record holder for the most number of aircraft flown (12) in parabolas, personally logging more than 7,300 parabolas.
\n\nSeeing the 5,000th book published makes us at the same time proud, happy, humble, and grateful. This is a great opportunity to stop and celebrate what we have done so far, but is also an opportunity to engage even more, grow, and succeed. It wouldn't be possible to get here without the synergy of team members’ hard work and authors and editors who devote time and their expertise into Open Access book publishing with us.
\n\nOver these years, we have gone from pioneering the scientific Open Access book publishing field to being the world’s largest Open Access book publisher. Nonetheless, our vision has remained the same: to meet the challenges of making relevant knowledge available to the worldwide community under the Open Access model.
\n\nWe are excited about the present, and we look forward to sharing many more successes in the future.
\n\nThank you all for being part of the journey. 5,000 times thank you!
\n\nNow with 5,000 titles available Open Access, which one will you read next?
\n\nRead, share and download for free: https://www.intechopen.com/books
\n\n\n\n
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health of the population. Enhancing public health is of significant importance to the development of a nation, particularly for developing countries where the health care system is underdeveloped, fragile or vulnerable.This book examines progress and challenges with regards to public health in developing countries in two parts: Part 1 “General and Crosscutting Issues in Public Health and Case Studies” and Part 2 “Country-Specific Issues in Public Health.” For example, assuring equity for marginalized indigenous groups and other key populations entails the application of transdisciplinary interventions including legislation, advocacy, financing, empowerment and de-stigmatization. The diverse structural, political, economic, technological, geographical and social landscape of developing countries translates to unique public health challenges, infrastructure and implementation trajectories in addressing issues such as vector-borne diseases and intimate partner violence.This volume will be of interest to researchers, health ministry policy makers, public health professionals and non-governmental organizations whose work entails collaborations with public health systems of developing nations and regions.",isbn:"978-1-78985-874-7",printIsbn:"978-1-78985-873-0",pdfIsbn:"978-1-83962-380-6",doi:"10.5772/intechopen.83134",price:119,priceEur:129,priceUsd:155,slug:"public-health-in-developing-countries-challenges-and-opportunities",numberOfPages:274,isOpenForSubmission:!1,hash:"28c7e86f71905feb65668941c4f259f4",bookSignature:"Edlyne Eze Anugwom and Niyi Awofeso",publishedDate:"September 9th 2020",coverURL:"https://cdn.intechopen.com/books/images_new/9138.jpg",keywords:null,numberOfDownloads:6784,numberOfWosCitations:0,numberOfCrossrefCitations:3,numberOfDimensionsCitations:13,numberOfTotalCitations:16,isAvailableForWebshopOrdering:!0,dateEndFirstStepPublish:"March 14th 2019",dateEndSecondStepPublish:"May 2nd 2019",dateEndThirdStepPublish:"July 1st 2019",dateEndFourthStepPublish:"September 19th 2019",dateEndFifthStepPublish:"November 18th 2019",remainingDaysToSecondStep:"2 years",secondStepPassed:!0,currentStepOfPublishingProcess:5,editedByType:"Edited by",kuFlag:!1,biosketch:null,coeditorOneBiosketch:null,coeditorTwoBiosketch:null,coeditorThreeBiosketch:null,coeditorFourBiosketch:null,coeditorFiveBiosketch:null,editors:[{id:"293469",title:null,name:"Edlyne Eze",middleName:null,surname:"Anugwom",slug:"edlyne-eze-anugwom",fullName:"Edlyne Eze Anugwom",profilePictureURL:"https://mts.intechopen.com/storage/users/293469/images/9729_n.jpg",biography:"Edlyne Anugwom is a Professor of Sociology and Development\nat the University of Nigeria and until recently Georg Forster\nSenior Research Fellow of the Humboldt Foundation at the\nInstitute of African Studies, Leipzig University. He has held\nteaching positions/fellowships in such diverse places as Leiden,\nWassenaar, Birmingham, Bridgewater, Edinburgh, Mainz, Cape\nTown, and others. His research interests are in the areas of social\nresearch, public health, political sociology of development, social conflict and terrorism in Africa. Significant publications include: Research Methods in Social Sciences\n(2010, Fourth Dimension Pub); The Boko Haram Insurgence in Nigeria: Perspectives\nfrom Within (2019, Palgrave Macmillan); From Biafra to the Niger Delta Conflict:\nMemory, Ethnicity and the State in Nigeria (2019, Lexington Books); and Development in Nigeria – Promise on Hold? (2020, Routledge). In addition, he has published\nmore than 100 peer-reviewed journal articles and as many book chapters.",institutionString:"University of Nigeria",position:null,outsideEditionCount:0,totalCites:0,totalAuthoredChapters:"2",totalChapterViews:"0",totalEditedBooks:"1",institution:{name:"University of Nigeria, Nsukka",institutionURL:null,country:{name:"Nigeria"}}}],coeditorOne:{id:"36610",title:"Prof.",name:"Niyi",middleName:null,surname:"Awofeso",slug:"niyi-awofeso",fullName:"Niyi Awofeso",profilePictureURL:"https://mts.intechopen.com/storage/users/36610/images/system/36610.jpeg",biography:"Niyi Awofeso is currently a professor at the School of Health and Environmental Studies Hamdan Bin Mohammed Smart University (HBMSU), Dubai. He commenced his public health career as an infectious disease physician and acting medical director at Nigeria’s National Tuberculosis and Leprosy Training Centre in 1990. Prior to joining HBMSU in 2013 from the University of Western Australia where he worked as Professor of Health Management, he accumulated extensive research and professional experience at both middle and senior management levels in academia and the international health industry. He holds postgraduate qualifications in infectious diseases medicine, public health, business administration and health administration. He has so far published more than 120 peer-reviewed articles in well-regarded academic journals, authored five books and eight book chapters.",institutionString:"Hamdan Bin Mohammed Smart University",position:null,outsideEditionCount:0,totalCites:0,totalAuthoredChapters:"2",totalChapterViews:"0",totalEditedBooks:"0",institution:{name:"Hamdan Bin Mohammed Smart University",institutionURL:null,country:{name:"United Arab Emirates"}}},coeditorTwo:null,coeditorThree:null,coeditorFour:null,coeditorFive:null,topics:[{id:"1131",title:"Global Health",slug:"global-health"}],chapters:[{id:"72687",title:"Introductory Chapter: Public Health Afflictions and Challenges in the Developing World",slug:"introductory-chapter-public-health-afflictions-and-challenges-in-the-developing-world",totalDownloads:172,totalCrossrefCites:0,authors:[{id:"293469",title:null,name:"Edlyne Eze",surname:"Anugwom",slug:"edlyne-eze-anugwom",fullName:"Edlyne Eze Anugwom"}]},{id:"69468",title:"The Global Burden and Perspectives on Non-Communicable Diseases (NCDs) and the Prevention, Data Availability and Systems Approach of NCDs in Low-resource Countries",slug:"the-global-burden-and-perspectives-on-non-communicable-diseases-ncds-and-the-prevention-data-availab",totalDownloads:1759,totalCrossrefCites:0,authors:[{id:"306689",title:"Dr.",name:"Melkamu",surname:"Kassa",slug:"melkamu-kassa",fullName:"Melkamu Kassa"},{id:"306691",title:"Dr.",name:"Grace",surname:"Jeanne",slug:"grace-jeanne",fullName:"Grace Jeanne"}]},{id:"69370",title:"Non-Communicable Diseases and Urbanization in African Cities: A Narrative Review",slug:"non-communicable-diseases-and-urbanization-in-african-cities-a-narrative-review",totalDownloads:563,totalCrossrefCites:2,authors:[{id:"304657",title:"Dr.",name:"Kenneth",surname:"Juma",slug:"kenneth-juma",fullName:"Kenneth Juma"},{id:"310042",title:"Dr.",name:"Gershim",surname:"Asiki",slug:"gershim-asiki",fullName:"Gershim Asiki"},{id:"310043",title:"Dr.",name:"Pamela",surname:"Juma",slug:"pamela-juma",fullName:"Pamela Juma"},{id:"310045",title:"Dr.",name:"Peter",surname:"Otieno",slug:"peter-otieno",fullName:"Peter Otieno"},{id:"310059",title:"Dr.",name:"Constance",surname:"Shumba",slug:"constance-shumba",fullName:"Constance Shumba"}]},{id:"71667",title:"Health Promotion and Its Challenges to Public Health Delivery System in Africa",slug:"health-promotion-and-its-challenges-to-public-health-delivery-system-in-africa",totalDownloads:559,totalCrossrefCites:0,authors:[{id:"293469",title:null,name:"Edlyne Eze",surname:"Anugwom",slug:"edlyne-eze-anugwom",fullName:"Edlyne Eze Anugwom"}]},{id:"72878",title:"Understanding the Science of Indigenous Health System: Key to Sustainable Collaborations",slug:"understanding-the-science-of-indigenous-health-system-key-to-sustainable-collaborations",totalDownloads:277,totalCrossrefCites:0,authors:[{id:"304220",title:"Prof.",name:"Simon",surname:"Nemutandani",slug:"simon-nemutandani",fullName:"Simon Nemutandani"}]},{id:"72270",title:"Public Health Effects of Wood Fuel in Africa: Bioenergy from Tree Commodities as a Sustainable Remedy",slug:"public-health-effects-of-wood-fuel-in-africa-bioenergy-from-tree-commodities-as-a-sustainable-remedy",totalDownloads:247,totalCrossrefCites:0,authors:[{id:"237109",title:"M.Sc.",name:"Serge Mandiefe",surname:"Piabuo",slug:"serge-mandiefe-piabuo",fullName:"Serge Mandiefe Piabuo"},{id:"310642",title:"MSc.",name:"Janice",surname:"Tieguhong Puatwoe",slug:"janice-tieguhong-puatwoe",fullName:"Janice Tieguhong Puatwoe"}]},{id:"69631",title:"Cultural Practices and Health Consequences: Health or Habits, the Choice Is Ours",slug:"cultural-practices-and-health-consequences-health-or-habits-the-choice-is-ours",totalDownloads:216,totalCrossrefCites:0,authors:[{id:"302308",title:"Dr.",name:"Radiance",surname:"Ogundipe",slug:"radiance-ogundipe",fullName:"Radiance Ogundipe"}]},{id:"70667",title:"Mitigating the Hazard of Lightning Injury and Death across Africa",slug:"mitigating-the-hazard-of-lightning-injury-and-death-across-africa",totalDownloads:281,totalCrossrefCites:0,authors:[{id:"183336",title:"Dr.",name:"Mary Ann",surname:"Cooper",slug:"mary-ann-cooper",fullName:"Mary Ann Cooper"},{id:"305781",title:"Mr.",name:"Ronald L.",surname:"Holle",slug:"ronald-l.-holle",fullName:"Ronald L. 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Local allergic rhinitis (LAR) is defined by symptoms suggestive of allergic rhinitis (AR), but with no detected sensitivity to an allergen using common allergy testing, while allergen-specific immunoglobulin-E (IgE) in the nasal mucosa can be detected.
\nThe first report of local production of IgE in the nasal mucosa was documented in 1975 among patients with typical symptoms of allergic rhinitis and negative allergy evaluation (i.e., negative skin prick tests (SPT) or serum-specific IgE (sIgE)). In this early report, specific IgE antibodies to
The prevalence of LAR is uncertain and was long considered a rare disorder. In recent years, with the improvement of diagnostic methods, new and surprising data has emerged. In 2012 Rondon et al. reported a prevalence of 25.7% of LAR among a group of 428 adult patients with chronic rhinitis. In the same cohort, 63.1% were diagnosed with AR and 11.2% with non-allergic rhinitis (NAR). The most frequently causative allergen in both LAR and AR was
As mentioned above, LAR has to be considered in the differential diagnosis of AR, when no evidence of systemic atopy is present. The evaluation of a patient suspected to have LAR should include a detailed clinical history, typically resembling AR, as well as assessment of comorbidities, such as ocular, skin, and bronchial symptoms. This may enable further evaluation for systemic atopy or a filter for patients with non-allergic rhinitis (NAR; see Table 1). A detailed physical examination includes inspection of the nasal cavity via nasal endoscopy, and for some patients, a CT scan may be required to exclude other causes of chronic rhinitis. This should be followed by tests to verify sensitization to aeroallergens, either skin prick tests (SPT) or serum-specific IgE. It has been suggested that when there is a high index of suspicion of allergy and no reaction to SPT, intradermal skin tests to common aeroallergens may be considered. In the absence of evidence for systemic sensitization, one must prove local rhino-mucosa hyper-reactivity to aeroallergens in order to diagnose LAR [6, 7] (Figure 1). Three methods can be used to diagnose LAR:
NAPT is a sensitive and specific technique, although it requires special training and is time-consuming [8]. Furthermore, it has some pitfalls. Nasal challenge with saline prior to NAPT is recommended to rule out non-specific nasal hyper-reactivity, which may induce a false-positive result. Having said that, there is yet lack of standardization regarding allergenic extract, dose, timing, and outcome definitions of NAPT [9].
In summary, BAT has a medium-grade sensitivity and a high specificity for the diagnosis of local sIgE, which may outperform other methods for sIgE detection. It is less time-consuming; however, it is performer dependent compared to NAPT.
\n
| \n
Differential diagnosis of allergic and local allergic rhinitis.
Allergic rhinitis diagnostic algorithm. SPT, skin prick test; ID, intradermal skin tests; sIgE, specific IgE; NAPT, nasal provocation test; BAT, basophil activation test.
The pathogenesis of allergic rhinitis (AR) is well established. It is a Th2-mediated disease which involves mast cell activation, recruitment of eosinophils, basophils and T cells expressing Th2 cytokines, and secretion of interleukin as IL-4, IL-13, IL-5, and others. The pathophysiology of LAR is less well established, and the question why the majority of allergic patients exhibit systemic sensitization (atopy) while some develop only local responses (entopy) is yet to be answered. Nonetheless, it has been suggested that the natural history of allergy is composed of multiple steps leading eventually to atopy. In a recent review, Dullaers et al. [13] suggested that the first step to atopy takes place in the nasal mucosa, where allergen-specific IgE is produced. The authors further hypothesized that some subjects lack spillover of these mucosal-produced allergen-specific IgEs into the circulation. In another study, the detection of allergen-specific IgE on the surfaces of peripheral basophils from patients with LAR eluded to the idea that the second step to atopy is on the surface of peripheral basophils and other target immune cells, followed by the third and final step which is the detection of serum-specific IgE and skin mast cell sensitization [12]. Thus, differences between LAR and AR may explain different stages of sensitization to allergen. For example, it was demonstrated that following nasal provocation of patients allergic to olive, the ECP levels in nasal lavage were significantly higher in both AR and LAR patients than in controls, while basophil activation test (BAT) was higher only in the LAR group, which potentially represents an earlier step in sensitization, associated more closely with LAR [14].
\nIn contrast, similarities between AR and LAR pathophysiology were observed while evaluating the immunologic responses to therapy and particularly to immunotherapy. Namely, alike AR patients a significant increase of serum-specific IgG4 antibodies is observed following allergen immunotherapy among LAR patients. This not only substantiates the IgE-mediated mechanism of disease but also the notion that LAR may be the prodrome of AR [15]. Last but not least, allergen-specific IgEs to various allergens in the nasal scrapings from patients with AR, non-allergic rhinitis (NAR), and healthy controls were reported to be 86.7, 33.3, and 50%, respectively. Thus, although a wide difference between allergic and non-allergic patients was documented, a relatively high percent of IgE production was observed among controls [16]. One may suggest that healthy controls were sensitized but developed spontaneous tolerance, e.g., “a backward step” following the first, second, or third stage of atopy.
\nAR is an essential part of the “atopic march” [17] and thereby associated with comorbidities, such as asthma, atopic dermatitis, food allergies eosinophilic esophagitis, allergic conjunctivitis, chronic rhinosinusitis with nasal polyposis (CRSwNP), and more [18]. The association of these comorbidities with local allergic rhinitis (LAR) was less explored [19], although bronchial symptoms have been reported in patients with LAR [20] and any chronic rhinitis is a risk factor for poorly controlled asthma with recurrent hospital visits [19]. Recently, self-reported bronchial symptoms, suggestive of asthma, were reported in over 30% of patients with LAR, suggesting a new asthma phenotype, “local allergic asthma” [21, 22]. As in classical allergic rhinitis, conjunctival symptoms were also associated with LAR. It was shown that patients with LAR experience ocular symptoms during nasal exacerbations due to allergen exposure or during in vitro nasal provocation tests [20]. In one study, this was the most prevalent comorbidity associated with LAR [23]. In a recent study by Rondon et al. [19], a 10-year follow-up of 176 LAR patients entailed other comorbidities, such as food allergy and drug hypersensitivity, which were documented only in few patients.
\nIn daily practice NAPT, BAT, or other specific tests are rarely performed. Hence, performing a therapeutic trial with antihistamines may be beneficial for diagnosis of LAR. Early and substantial response to antihistamine further supports an allergic histamine-driven mechanism. In the same line of thought, treatment with nasal corticosteroid spray may be clinically beneficial, but will not enable to differentiate causes of chronic rhinitis. Most LAR patients are currently treated similarly to AR patients, and according to the allergic rhinitis and its impact on asthma (ARIA) guidelines. This is done by using personal and environmental education, allergen avoidance measures and non-specific pharmacologic modalities, such as, intranasal corticosteroids, and oral and intranasal antihistamines [7, 8, 9, 10]. Having said that, such non-specific therapy for LAR will ameliorate symptoms but alike AR will not change the natural progression of disease.
\nImmunotherapy is a common therapeutic modality for moderate to severe unresponsive AR. Allergen immunotherapy is based on gradual exposure to a culprit allergen via subcutaneous or sublingual exposure. This will eventually result in “induced tolerance” to the targeted allergen and amelioration of the allergic response. Allergen immunotherapy is highly effective and safe and confers long-term clinical benefit in adequately selected patients. Furthermore, it is the only etiological treatment for AR and asthma which conveys disease-modifying effect that can actually change the natural course of the disease [8, 9]. Thus, although LAR is by definition a local rather than systemic disease, few studies provide evidence for clinical benefit of allergen immunotherapy among LAR patients. These studies demonstrated a significant symptom improvement, an increase in the number of medication free days, and a beneficial effect on ocular symptoms, asthma control, and quality of life compared to placebo, as well as tolerance induction defined by an increase in allergen-specific IgG4 [6, 7, 8, 10].
\nIn the last decade, growing evidence indicates that nasal reactivity to aeroallergens can occur in the absence of evidence of systemic atopy. The published literature raised the suspicion that many patients diagnosed previously as suffering from non-allergic rhinitis actually suffer from LAR. This may be of importance as treatment options differ between non-allergic and AR/LAR diseases. Diagnosis of LAR remains a challenge, as none of the diagnostic methods suggested are optimal nor commonly available in most centers. Therefore, high index of suspicion, utilizing specific methods if accessible as well as therapeutic challenge, may enable correct and early diagnosis. This may enable specific allergen-directed interventions (e.g., allergen immunotherapy), as well as early detection and treatment of comorbidities (like asthma and conjunctivitis). In this regard, implementation of NAPT, BAT, and other methods of diagnosis, especially in referral centers, as well as long-term studies to better define the mechanisms, course, and response to therapy of LAR, is needed.
\nUnregulated emerging pollutants enter aquatic systems through wastewater treatment plants after consumption and use by humans and animals [1].
This poses a significant risk to aquatic organisms and to public health. Among the main effects described to date are the appearance of changes in fish reproduction due to the presence of hormones and inhibition of photosynthesis in algae by the presence of these [2]. We know that the presence of antibiotics in the environment can make bacteria in wastewater relatively more resistant to them and resistant microorganisms develop.
To make clear how these molecules act as endocrine disruptors, we must indicate that they interfere with the body’s homeostasis, usually by mimicking the natural hormones that lead to the activation or blocking of their receptors [3].
Trimethoprim in Mexico is one of the most used drugs for treating urinary tract infections, and it is commonly used in the foreign tourism for attending the traveler’s diarrhea [4]. Trimethoprim is incompletely metabolized by humans during the therapeutic process and approximately 80% is excreted in the pharmacologically active form, which can promote the development of bacterial resistance to this compound’s form promoting it as an emerging contaminant [5].
Clavulanic acid-amoxicillin is a mixture of two drugs in typical commercial compositions of 185/125 and 500/125 mg and commercially known in México as Augmentin and Clamoxin or Gimaclav, respectively. It is indicated for the treatment of acute and chronic infections of the upper and lower respiratory tracts, meningitis and genitourinary, skin, soft tissue, gastrointestinal and biliary infections, and in general for the treatment of infections caused by pathogens sensitive to this mixture of drugs [6].
Both drugs have been studied by our research group as emerging pollutants with an effect of endocrine disruptors due to their high presence in wastewater of domestic and hospital effluents in México (work in process of being published) and their consequent impact on all types of aquifers, which could act as final receiving bodies. However, in our research group, different advanced oxidation processes have been used and improved for the removal of these kinds of contaminants, these processes include cavitation, photo-catalytic oxidation, or Fenton chemistry, but they have high costs. New expectations were found when it has been applied an electrochemical process.
Electrochemical oxidation is based on the application of an electric current or a potential difference between two electrodes (anode and cathode), wherewith hydroxyl radicals or other oxidizing species can be generated, depending on the anode material used and the type of electrolyte support used [7].
In this chapter, the use of electrolysis for the removal of pharmaceutical-type pollutants is based on the chemical reactions that are carried out between the electrodes submerged in electrolytic solutions by effect of the passage of the electric current, being the function of the electrolyte to serve as a means of transporting electrical loads and provoke the reactions of oxidation-reduction for the degradation of compounds in order to transform them into less hazardous compounds for the environment. The electrolyte being of the family of salts allows the anions to carry negative loads toward the anode and the cations transport the positive loads to the cathode [8]; the effectiveness of several visible light-activated TiO2 photocatalysts has been proven for the treatment of emerging contaminants. Doping or co-doping of titanium dioxide using nitrogen, nitrogen-silver, sulfur, carbon, and copper and incorporating graphene nano-leaves increases its effectiveness. The use of titanium dioxide is to improve photocatalytic activity [9]. Considering all the above backgrounds, the experiments reported hereby were performed in order to establish if the proposed system could breakdown or transform the pollutants (drugs) into simpler molecules.
Based on different references, it is known that the trimethoprim can be determined with an absorbance at 237.6 nm [10] or that it can be displayed at a wavelength of 283–350 nm [11], and it is mentioned that in visible light, it is still observed at a wavelength between 400 and 600 nm [12]. In the case of amoxicillin-clavulanic acid mixture, the spectra recorded are in a wavelength range of 200–380 nm [13]. Therefore, the results on the UV-Vis spectrum were analyzed within these intervals.
For the preparation of synthetic wastewater (SWW) contaminated by trimethoprim and clavulanic acid-amoxicillin, three samples with 500 mL of clean water (0.1 mS/cm) were added with different drug concentrations (trimethoprim 0.1%, trimethoprim 0.2%, and clavulanic acid-amoxicillin 0.2%). Type curves for each drug were prepared with 2 g/L (0.2%) as the highest concentration and 0.1 g/L (0.01%) as the lowest concentration.
The drugs supplied by Merck | Sigma-Aldrich were white powders, and the solutions prepared were kept in refrigeration (6°C) until needed.
For the construction of the electrodes, two glass tubes were used, each one of 6.1 cm length and 0.7 cm width, containing the following elements: an electrode connected to the negative pole (cathode) was handcrafted with mineral carbon introducing a copper wire (0.3 mm Ø) and the electrode connected to the positive pole (anode) was also handcrafted with mineral carbon doped with TiO2 and it was used a platinum wire (0.1 mm Ø). In the cathode, the reduction processes take place and oxidation occurs in the anode, where both are connected to a power supply with a 5 V electrical potential (Figure 1).
TiO2-doped electrodes and coal.
Platinum is an inert metal that does not participate in the redox reaction but only exchanges electrons [14] since it has a low reactivity with oxygen and with water [15]. Copper is a metal with great ductility and high electrical conductivity [16], which leads to the conclusion that both metal wires are good conductors and will show little corrosion. Furthermore, platinum has catalytic activity and low reactivity. Due to these characteristics, the platinum and copper wires were selected for the electrodes. Doping carbon with TiO2 aids a better oxidation process at the anode, in addition to having photocatalytic properties that can improve the dissociation reaction in the electrolytic cell.
The mineral coal was obtained from zinc-carbon battery carbon cylinders free of cadmium (0% Cd) and (0% Mg) magnesium, confirmed by atomic absorption; so, the mineral coal is free of these elements. Extracted amounts were obtained from different brands of batteries (MARKS rocket, explosive, Panasonic super hyper, King Kong, Sony-new ultra, and Kodak extra heavy-duty, among others). The cylinders were washed by immersion overnight (almost 8 hours) and rinsed with deionized water type I. The zinc and manganese content were also analyzed by atomic absorption of all the carbon cylinders obtained; determination of ammonium chloride was also performed but in the remaining rinse water used to clean the cylinders (the chlorides were quantified by the Mohr method and ammonia by the selective electrode method). Curiously after washing and rinsing the carbon cylinders, the concentrations of zinc and ammonium chloride were not detectable and there is only less than 0.1% impregnation of manganese, which was considered negligible for the experiment.
The coal cylinders were divided into two portions, one was ground directly and the other portion was doped with TiO2 and ground.
The mineral carbon was added into a TiO2 solution at 3.46 g/L (3.46%) and after that it was introduced to a stove at 100°C for approximately 2 hours. Finally, the mineral carbon doped with TiO2 was crushed, until a homogenous fine powder (0.65–1 μm) was obtained.
Having prepared both coals (doped and not doped), the glass cylinders were filled separately with them and the copper and platinum wires were placed along leaving 7.5 cm of free wire.
To assemble the electrochemical cell, it was designed with an acrylic cell, a power supply (5 V DC) from STEREN, a porous rectangle glass membrane (length 8.5 cm, height 3.8 cm, and width 7.0 mm), and the handcrafted electrodes. For the proper functioning of the electrolyte cell, moving of charges from the anode to the cathode and to balance the aqueous solution, a KOH electrolyte (0.01 M) from Merck | Sigma-Aldrich was used. The experiments were performed using 50 mL of the mentioned electrolyte solution and about 200–240 mL of SWW, inside the cell. All the experiments were performed in triplicate.
Twenty milliliters of samples of treated synthetic wastewater (TSWW) were taken every half an hour for an experimentation time period between 1.5 and 2 hours, and at time 0, intermediate and final time samples were collected for each experiment. Parameters such as pH, conductivity, and temperature for each sample were measured. A Hach brand Pro HR pocket conductivity tester was used; the temperature is given in °C and the conductivity in mS/cm.
Determination of total organic carbon (TOC) was performed for all the samples using a Thermo Scientific HiperTOC using the US standard US EPA 415.3. Another analytical method performed also for all the samples was the chemical oxygen demand (COD) under the Mexican Standard NMX-AA-030/2-SCFI-2011. Both methods were carried out by an IPN reference laboratory, which is certified by the Mexican Accreditation Entity (MAE). Also, each sample was taken for analyzing with thin layer chromatography (TLC) and UV-Vis spectrometry analysis at different wavelengths.
A visible ultraviolet spectrometer BECKMAN brand model DU 7500i was used for the UV-Vis spectrometry technique. First, an absorbance sweep was performed with the SWW samples at different concentrations, in order to find the highest absorbance wavelength to perform their type curves for both drugs. Subsequently, each of the TSWW samples was also measured at a wavelength ranging from 200 to 350 nm (UV absorbance) and 400 to 800 nm (Vis absorbance) in order to observe the degree of degradation or breakage that was achieved.
In order to validate the analytical methodology, the technical guide on traceability and uncertainty is used with those analytical measurements performed with an ultraviolet-visible spectrophotometry technique, which supports the application of the NMX-17025-IMNC-2006 standard, the foregoing established by the National Metrology Center (NMC) and the Mexican Accreditation Entity (MAE) [17].
For thin-layer chromatography, a 2.5 cm by 4 cm thin gel plate was used as a stationary phase; also, both drug standards from Merck | Sigma-Aldrich, two glass chromatographic cameras, and a 254 nm wavelength UV frame were needed. Polar and non-polar (intermediate) solutions were used as mobile phases (eluents). The polar and non-polar (intermediate) eluent solutions were prepared with different concentrations of hexane and ethyl acetate, both from chromatographic grade (Merck | Sigma-Aldrich). The non-polar (intermediate) contained a 4:6 ratio of ethyl acetate and hexane. The polar eluent does a 6:4 ratio of ethyl acetate and hexane. The TSWW samples were mixed with ethyl acetate in a 4:3 ratio inside a test tube and agitated for 30 seconds.
From the test tube, an aliquot of the TSWW samples was taken with a capillary. For each experiment, the TSWW samples were taken at the start, intermediate, and final times, the aliquots were placed subsequently on the thin plate, and the plate was introduced to the chromatographic chambers each with a different eluent (polar and non-polar). After taken out from the camera, plates were revealed under the 254 nm ultraviolet light. The running fronts for standards and sample components were calculated. The intention to use this method is because it is applied in the pharmaceutical industry as a compound purity determination. Therefore, with this technique, it has been able to see qualitatively whether there is a decrease or breaking of the contaminants in the TSWW sample compared against a SWW sample.
The model designed and constructed for the electrolytic cell used in the breakdown of the trimethoprim and acid clavulanic-amoxicillin is described in Figure 2.
Main components of an electrolytic cell.
The type curves for both drugs that were obtained and are showed in Figures 3 and 4 with their corresponding equations and linear coefficient.
Type curve of trimethoprim at a wavelength of 300 nm.
Clavulanic acid-amoxicillin type curve with a wavelength of 300 nm.
Eq. (1) shows the linearity, for the trimethoprim.
Equation (3) shows the linearity for the acid clavulanic.
The results obtained from the UV-Vis spectrometry technique at 350 nm is shown in Figure 5 and results with a 400 nm wavelength is shown in Figure 6, where the absorbance units were plotted with respect to the treatment time. When handling a compound that has rings and double bonds in its molecular structure, it is able to absorb ultraviolet light, and according to the Lambert-Beer law, the absorbance of a substance is proportional to the concentration of the compound.
Mean absorbance decreasing of trimethoprim at different treatment times, at a wavelength of 350 nm.
Absorbance units of the clavulanic acid-amoxicillin mixture at different treatment times, at a wavelength of 400 nm.
From the graphs above, we can observe a decay of the absorbance in the trimethoprim at 90 minutes and an increase in the clavulanic acid-amoxicillin mixture experiment after 30 minutes of treatment. These results indicate that there is surely a breakdown in both molecules, but the structure of the molar fragments for trimethoprim differs with respect to the clavulanic acid-amoxicillin mixture. In the first one, the absorbance decreases, but in the second, it increases. It is known that the molecules whose absorbance decays in an electrochemical process present a process of chemical reduction (electron gain), while the compounds whose absorbance increases are understood to undergo chemical oxidation processes (loss of electrons).
For the clavulanic acid-amoxicillin mixture, the increase in absorbance may be due to structural changes in the molecule, so the chemical structure was modified during the reaction, generating resonance systems that will show higher absorbances. Furthermore, this increase in absorbance may be due to the formation of other compounds in the electrolysis reaction, such as hydrogen near the cathode and oxygen near the anode. In the disintegration of water, both ozone and hydrogen peroxide are formed in small quantities [18]; it is known that ozone strongly absorbs radiation in the infrared, visible, and ultraviolet regions [19]. The maximum absorption occurs at a wavelength of 253.7 nm [19], which can be observed in the scanning of the spectrophotometer in Figure 7. For these experiments, the wavelength was taken at 400 nm because the sample presented a light yellow hue coloration, which may be due to the fact that the spectral properties of organic molecules depend on the type of valence electrons, on their quantum possibilities of absorption of UV-Vis radiation, and on the presence of chromophoric groups in their structures [20]; therefore, the sigma (σ) electrons make up the single saturated bonds or molecular bonding orbitals of the sigma type, while the pi (π) electrons make up the multiple unsaturated bonds or pi orbitals. These unsaturated groups are called chromophoric groups [21]. The appearance of color in some organic substances is related to the presence of one or more chromophoric groups whose pi electrons are easily excited by the absorption of radiation from the near and visible ultraviolet region (200–800 nm), of corresponding energy (specific length) to the quantum possibilities for the electronic transition [21]. Therefore, it is not certain that in the case of the clavulanic acid-amoxicillin mixture, there is an adequate decomposition, but for the trimethoprim component, this degradation is observed.
Full scan of the UV-Vis spectrometer for samples at different treatment times of the clavulanic acid-amoxicillin mixture.
The electrical conductivity is in correlation of the amount of ionizable molecules or radicals present in the water as shown in Figures 8 and 9; as time passes, conductivity increases, meaning that the drug molecules are being broken and more ionizable fragments are generated.
Conductivity against time for experiments with trimethoprim.
Conductivity against time for experiments with the clavulanic acid-amoxicillin mixture.
The COD graph that was obtained from the Trimethoprim TSWW samples showed a tendency to decrease according to the time elapsed. The initial COD at time 0 for the first experiment (trimethoprim 0.2%) had a concentration of 199.1 mg/L and the second experiment (trimethoprim 0.1%) had the lowest drug concentration of 90.3 mg/L of COD; you can see that in 1 hour, the COD concentration of the first trimethoprim 0.2% experiment dropped to 142.8 mg/L, and in the second experiment, it dropped to a concentration of 88.5 mg/L. This shows that the degree of contamination of the water by organic compounds (TSWW) decreases, that is, the organic matter (drug) decreases, and therefore there is a break in the contaminant.
It is also observed that in the second experiment (trimethoprim 0.1%), there is a slightly lower concentration of drug and that when passing through the electrolysis treatment it presents a greater removal efficiency, since the COD decreases more as time passes, compared to the trimethoprim 0.2%, which has a slight increase and decay (Figure 10).
Chemical oxygen demand with respect to time.
The results of total organic carbon can be seen in Figure 11. It is observed in the graph that there is a tendency to decrease the concentration of carbon as time goes by. The initial TOC of the first experiment had a concentration of 98.5 mg/L and the second experiment had an initial concentration of 59.4 mg/L. In both cases, from the 30th minute on, it is observed that trimethoprim 0.2% decreases to a concentration of 56.5 mg/L and trimethoprim 0.1% to a concentration of 33.5 mg/L. The above proves that the electrolytic system is an alternative for trimethoprim decomposition.
Total organic carbon with respect to time.
Table 1 shows that during the electrolytic breakdown, carbon portions are mineralized but some fragments must have been ionized in different forms that affects the UV-Vis absorbance.
TOC (mg/L) | |
---|---|
Trimethoprim 0.2% | Trimethoprim 0.1% |
98.5 | 59.4 |
90 | 53.9 |
71.6 | 45.2 |
67.4 | 40.8 |
56.5 | 33.5 |
Total organic carbon results from experiments 1 and 2 with trimethoprim.
Finally, Table 2 shows the maximum percentage of degradation that was obtained from the synthetic wastewater when it was treated with the electrolytic cell, for the first and second experiments with trimethoprim.
%Degradation according to TOC | |
---|---|
The first experiment (trimethoprim 0.2%) | The second experiment (trimethoprim 0.1%) |
91.3706 | 90.7407 |
Maximum percentages of degradation obtained from TSWW samples with electrolysis treatment.
In the case of the clavulanic acid-amoxicillin TSWW mixture, the COD had an oscillating behavior because at 1 minute it began to decrease and at 60 minutes it abruptly increased and then it decreased again. The initial COD at time 0 for the clavulanic acid-amoxicillin TSWW sample (0.2%) has a concentration of 266.5 mg/L, after 30 minutes, there is a concentration of 257.3 mg/L, but it is observed that at 60 minutes, the COD concentration abruptly increased to 261.2 mg/L. This experiment ended his treatment with a concentration of 242.3 mg/L. According to the bibliography analyzed, the phenomenon obtained in Figure 12 by the clavulanic acid-amoxicillin (TSWW) mixture could be due to the fact that when the sample is subjected to radiation, the molecule fragments and groups with free electron pairs are exposed and they absorb more radiation, generating increase in the values obtained. These formed fragments absorb a greater amount of energy after 60 minutes and as they continue to degrade and lose this capability.
Chemical oxygen demand against to time.
The total organic carbon (TOC) results for clavulanic acid-amoxicillin TSWW can be seen in Figure 13; there is a tendency to decrease the carbon concentration as time passes. The initial TOC of the clavulanic acid-amoxicillin TSWW mixture had a concentration of 182.8 mg/L and drops to a concentration of 164.6 mg/L. The above indicates the decrease in the sample of organic compounds due to the breakdown of the organic molecules to molecules with simpler structures.
Total organic carbon over time.
The results from the clavulanic acid-amoxicillin mixture experiments presented for the UV-Vis spectrophotometric studies give negative absorbance values, which is observed in Figure 6, probably due to the effects of the breakage of the molecule by chemical changes suffered in its structure, which generated ions or fragments with higher absorbances. This is because UV-Vis spectrophotometry excites the free electrons of oxygen, nitrogen, and sulfur that are present in both molecules, just as the molecule contains double bonds in its structure. In the pi bond, the electrons are excited and migrate to a higher energy level, modifying the structure. Therefore, the TOC was not used because negative values were being given in the absorbance.
The results of the clavulanic acid-amoxicillin mixture experiments presented for UV-Vis spectrophotometric studies in Figure 6 give high absorbance values, probably due to the effects of the breakdown of the molecule due to the electrochemical changes suffered in its structure, whereby ions or fragments with higher absorbances are generated. The modification of its structure is due to the fact that UV-Vis spectrophotometry excites the oxygen, nitrogen, and sulfur free electrons that are present in both molecules, as well as the pi electrons of the conjugated double bonds in its structure. In the pi bond, the electrons are excited but they can be delocalized by resonance effects, modifying the energy absorbed by the structure.
During the reaction, the formation of free radicals like HO• could occur, which are species with high reactivity, which allows them to attack organic molecules. It is worth mentioning that the photochemical process is not developing in the electrolytic cell, despite the fact that TiO2 reacts with light.
For the thin layer chromatography (see Figure 14), it is observed that there is a change of displacement between the 0 time and 60 minutes of the experiment. That is, the RF pattern for both drugs is not observed in comparison with the standards of trimethoprim and clavulanic acid-amoxicillin mixture; this indicates that the molecules at 60 minutes do not present the same structure. This is an expected result because in an electrolytic cell when an electric potential is applied, it generates an electric current passage, which is a flow of electrons between the electrodes creating a circuit of ionic and electric charges transport, besides getting the help of the electrolyte that maintains a balance of charges, which improves the transport of the charges between electrodes, causing the oxidation of fragments of the molecule in the surface of the anode and a reaction of reduction of other fragments of the molecule in the cathode.
Results of the thin layer chromatography demonstrating the rupture or breakdown of trimethoprim as also in the clavulanic acid-amoxicillin mixture, in which a great modification is observed, being less polar the product obtained with the treatment.
In addition, the electrode that is doped with titanium dioxide generates a greater oxidative effect, debt to its catalytic properties and the mineral carbon, has a porous structure and a large contact surface, and allows an adsorption process to take place between the organic compounds and the mineral carbon. Another advantage of using charcoal is that the problem of forming products that may be toxic does not arise, due to its high absorption capacity as mentioned before, although its efficiency may depend on the amount of material organic present in the solution.
The electrolyte cell demonstrated based on the results that it has the feasibility of breaking or/and debugging emerging endocrine disrupting contaminants like trimethoprim. The work developed by Sirés et al. in 2005 on the electrochemical degradation of water acetaminophen by catalytic action of Fe2+, Cu2+, and light showed that the acidic aqueous solutions of the drug acetaminophen were degraded by anodic oxidation in an undivided electrolytic cell with a Pt anode and an O2 supply [22], proving that the electrolysis process is functional. However, the materials and reagents to be used in this project are cheaper, and for a process tested in a single drug, there is no certainty how it will work in others.
Hirose et al. applied electrolysis for degradation of epirubicin, bleomycin, and mitomycin C with Pt/Ir electrodes and a NaCl solution as electrolyte. The results obtained were a partial degradation of the antibiotics but their cytotoxic and mutagenic activity was absolutely eliminated [23].
This research establishes that an elimination or rupture of different drugs can be carried out with an electrolytic cell, based on the work performed by Giraldo Aguirre et al. in 2016 on the electrochemical treatment of waters containing β-lactam antibiotics, where by means of electrolysis, the degradation of the drugs oxacillin (OXA), cloxacillin (CLX), and dicloxacillin (DCX) was achieved. Those drugs are also used as antibiotics [7] like trimethoprim and the clavulanic acid-amoxicillin mixture and can affect aquatic systems and health due to the fact that antibiotics are among the most consumed and released drugs to the environment [24]. This release is also due to the unwarranted prescription with antibiotics, its inadequate dispensing, and the laxity in the regulation on the sale of medicines that allows self-medication with antibiotics, which are some of the factors that have been related to this high consumption [24] because it is a chemically defined substance capable of modifying the biochemical and physiological activity in an organism and therefore can produce a biological, beneficial, or toxic effect depending on the dose delivered [25]. Another problem is based on worldwide studies that have evidenced the presence of pharmaceutical compounds in effluents from fully operational treatment plants and with their respective control parameters, apparently operating with a high wastewater purification efficiency [26]; so, it is now known that with conventional wastewater treatments, it is not possible to eliminate this type of compounds in an efficient level [26], having as a consequence the proliferation of bacteria resistant to antibiotics, which will cause major problems in aspects of public health. In the research of Giraldo Aguirre et al. [7], a Ti/IrO2 electrode was used which led to the oxidation process being better, which is due to the characteristics already mentioned for titanium and oxygen; also, the electrolyte that used sodium chloride helped them in the inhibition of microbial activity. This is because during the electrolysis reaction, chlorine gas is released from the electrolyte, but in our case, potassium hydroxide was used with the intention that the system can be incorporated to a wastewater treatment plant, since this technology usually uses biological reactors; therefore, only the breakdown of the molecule was sought without affecting the bio-catalytic bacteria during the subsequent processes. However, Giraldo Aguirre et al. conclude that electrochemical oxidation induces structural changes in antibiotic molecules and their results also indicate that electrochemical treatment is an effective technique for reducing the antibiotic potential that these compounds present, reducing the environmental risk due to the proliferation of bacteria resistant to antibiotics [7]. The aforementioned was also demonstrated within our experimentation when observed the graph of total organic carbon for the two experiments with trimethoprim and the thin layer chromatography for results with the clavulanic acid-amoxicillin mixture. This helps us show that the systems that use electrolysis break these compounds down into compounds that are less harmful to organisms and the environment. This experiment ends up being an important contribution to science in drug treatment and for a later use of electrolytic cells at higher levels, in addition to being highly versatile and to some extent economical oxidation processes.
The electrolytic cell modifies the structures of both molecules through different mechanisms, but in functional aspects, the electrolytic cell achieves the efficient degradation of trimethoprim unlike the clavulanic acid-amoxicillin mixture. It is established that the electrolytic cell can degrade some molecules more easily than others; so, we can establish that those compounds with a structure similar to trimethoprim could be degraded efficiently. However, it is also shown that to achieve the degradation of other compounds, it is necessary that the conditions of the electrolytic cell are adjusted again.
Addressing the problem of emerging pollutants that are endocrine disruptors is something really important and urgent, due to the impact they have not only on the environment but also on the health of living beings; so, it is important to transform them into less dangerous compounds for environment. Unfortunately, the methods of removing these contaminants are now expensive. That is why the implementation of the electrolytic cell is intended to create an economical option for the possible removal of these compounds, as it was shown to have a good degradation rate of trimethoprim. However, in the case of the clavulanic acid-amoxicillin mixture, it is necessary to modify its operating conditions.
All the authors appreciate the financial support given by the Instituto Politécnico Nacional (IPN) through the projects: SIP 20181685, SIP 20180081, and SIP 20190101.
The authors declare no conflict of interest.
nm | nanometer |
ml | milliliter |
μm | micrometric |
L | liter |
g | gram |
min | minute |
Abs | absorbance |
ECED | emerging contaminants endocrine disruptors |
TOC | total organic carbon |
COD | chemical oxygen demand |
Redox | reduction-oxidation reaction |
V | volts |
SWW | untreated synthetic waste water |
STWW | synthetic wastewater with treatment |
TLC | thin-layer chromatography |
mS | millisiemens |
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