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Photooxidation of Neonicotinoids (Imidacloprid) in Aqueous Solution by Vacuum UV Induced Advanced Oxidation Process

dc.contributor.advisorSanin, Selim Latif
dc.contributor.authorDerin, Halil
dc.date.accessioned2021-10-13T08:16:49Z
dc.date.issued2021
dc.date.submitted2021-02-02
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dc.identifier.other10380138
dc.identifier.urihttp://hdl.handle.net/11655/25552
dc.description.abstractAnthropogenic activities have caused pollutions of water sources with organic micro pollutants most of which are recalcitrant and not easily degradable in nature. In recent years, such pollutants have been frequently detected in various water sources and are considered to be one of the major threats to water quality. Among organic micro pollutants, imidacloprid which is the first introduced neonicotinoid insecticide and the most commonly used one, receives a high attention since its widespread presence in water bodies and persistence to conventional biological and chemical water/wastewater treatment methods. Imidacloprid pollution of aquatic systems has been found in several countries. Advanced oxidation processes (AOPs) has been successfully applied to oxidize recalcitrant organic pollutants in water and wastewater treatments. Vacuum ultraviolet (VUV) based AOP has gained attention in recent years to treat organic contaminants in water. Unlike to other AOPs, VUV irradiation is capable of generating hydroxyl radicals in water without addition of oxidants and catalysts. Primary goal of this doctoral study was to investigate effectiveness of VUV process on the degradation of imidacloprid in water. Additionally, effects of various experimental parameters, flow rate, initial pH of solution, initial imidacloprid concentration, presence of inorganic ions (HCO3-, CO32-, NO3-), water matrix, presence and absence of dissolved oxygen on the VUV induced photooxidation of imidacloprid was investigated. Independent performance verification of the VUV process was executed by discoloration of commercially available reactive textile dyes (Synozol Red KH-L and Synozol Yellow KH-L) in water. Effects of sleeve materials (clear fused quartz and high purity synthetic quartz) were also investigated during the discoloration study. The results showed that imidacloprid and reactive textile dyes were rapidly degraded by the VUV process. pH of the experimental solution played an important role in the degradation of imidacloprid by the VUV process. Significant decrease (15.33%) in the rate of degradation of imidacloprid was observed at basic pH=11 condition. Presence of inorganic ions (HCO3-, CO32-, and NO3-) also noticeably impacted the decomposition of imidacloprid via VUV photons. Among the experimental parameters water matrix affected the VUV photooxidation of imidacloprid the most due to presence of natural organic matters (NOM). Nevertheless, complete imidacloprid reduction was attained in less than 5 minutes of reaction time even in the presence of inorganic ions and natural organic matters. It was found that presence of dissolved oxygen did not have a significant impact on the degradation and mineralization processes. Kinetic analyses showed that degradation of imidacloprid by the VUV process under the all tested experimental conditions followed a pseudo first order reaction kinetic. Observed reduction rate constants of imidacloprid (Co = 5 mg/L) depending on the experimental conditions varied between 1.3877 min-1 and 1.9213 min-1. Almost 80% of 10 mg/L imidacloprid was mineralized by the VUV process within 2 hours of irradiation. LC/MS Q-TOF analyses revealed the generation of several byproducts during the VUV induced photooxidation of imidacloprid. Separate hydrolysis experiments revealed that imidacloprid was very stable under acidic (pH=3) and natural (original, pH=6.469) conditions during 104 days of hydrolysis time. Hydrolytic degradation of imidacloprid significantly increased under tested basic (pH=11) condition. First order kinetic pattern with the hydrolytic rate constant of 0.0083 day-1 and half-life of 83.51 days was observed at the tested alkaline solution. Additionally, it was found that Synozol Red KH-L and Synozol Yellow KH-L were also effectively removed by the VUV process. Textile dye experimental results showed that purity of the quartz sleeve used in the VUV photooxidation system had significant impact on the discoloration efficiency.tr_TR
dc.language.isoentr_TR
dc.publisherFen Bilimleri Enstitüsütr_TR
dc.rightsinfo:eu-repo/semantics/openAccesstr_TR
dc.subjectOrganic micro pollutants,tr_TR
dc.subjectImidacloprid
dc.subjectNeonicotinoids
dc.subjectVUV irradiation
dc.subjectAdvanced oxidation process
dc.subjectPhotooxidation
dc.subjectHydroxyl radicals
dc.subjectHydrolytic degradation
dc.subjectSynozol Red KH-L, and Synozol Yellow KH-L
dc.subject.lcshÇevre mühendisliğitr_TR
dc.titlePhotooxidation of Neonicotinoids (Imidacloprid) in Aqueous Solution by Vacuum UV Induced Advanced Oxidation Processtr_TR
dc.title.alternativeSu Ortamında Bulunan Neonikotinoidlerin (İmidakloprid) Vakum UV Işık İle Tetiklenen İleri Oksidasyon Prosesleri ile Giderimi
dc.typeinfo:eu-repo/semantics/doctoralThesistr_TR
dc.description.ozetAntropojenik faaliyetler, çoğu inatçı olan ve doğada kolayca parçalanamayan organik mikro kirleticilerle su kaynaklarının kirlenmesine çeşitli yollarla neden olmuştur. Son yıllarda, organik mikro kirleticiler çeşitli su kaynaklarında sıklıkla tespit edilmekte ve su kalitesine yönelik en büyük tehditlerden biri olarak kabul edimektedir. Organik mikro kirleticiler arasında, ilk piyasaya sürülen ve en yaygın kullanılan neonikotinoid insektisit olan imidakloprid, su kaynaklarında yaygın bir şekilde bulunmasından, geleneksel biyolojik ve kimyasal su ve atıksu arıtma yöntemlerine karşı dirençli olmasından dolayı su kaynaklarının korunması açısından büyük ilgi görmektedir. Yüzey ve yeraltı sularının imidakloprid kaynaklı kirliliği birçok ülkede tespit edilmiştir. İnatçı organik kirleticilerin su ve atıksudan gideriminde ileri oksidasyon prosesleri (İOP) başarıyla uygulanmaktadır. Vakum ultraviyole (VUV) bazlı ileri oksidasyon süreci, bu tür kirleticilerin sudan gideriminde etkinliğinden dolayı, son yıllarda dikkatleri üzerine çekmiştir. Diğer İOP’den farklı olarak, VUV ışıma herhangi bir oksitleyici ya da katalizör ilavesine gerek duymaksızın çok kuvvetli bir oksitleyici olan hidroksil radikallerini su ortamında oluşturabilmektedir. Bu doktora çalısmasının birincil amacı, VUV ışımanın imidaklopridin sudan giderimi üzerindeki etkinliğini tespit etmektir. Ayrıca, akış hızı, çözeltinin başlangıç pH’ı, imidakloprid başlangıç konsantrasyonu, inorganik iyonların varlığı, su matrisi, ve çözünmüş oksijenin varlığı gibi çeşitli deneysel parametrelerin imidaklopridin VUV ile fotooksidasyonu üzerindeki etkileri arastırılmıştır. VUV ışımanın bağımsız performans doğrulaması ticari olarak temin edilebilen reaktif tekstil boyalarının (Sinozol Kırmızı ve Sinozol Sarı) sudan arıtılmasıyla gerçekleştirilmiştir. VUV ışımada kullanılan kılıf malzemelerinin (berrak erimiş kuvars ve yüksek saflıkta sentetik kuvars) kirleticilerin sudan giderimine olan etkileri de bu doktora calışması kapsamında araştırılmıştır. Sonuçlar, imidakloprid ve reaktif tekstil boyalarının incelenen tüm deneysel parametreler altında VUV ışıma ile sudan hızlı bir şekilde giderildiğini göstermiştir. Çözelti pH’ı imidaklopridin VUV ışıma ile bozunumunda önemli bir rol oynamıştır. Bazik (pH=11) koşullar altında imidaklopridin bozunma oranında önemli düşüş (15.33%) gözlenmiştir. İnorganik iyonların (HCO3-, CO32- ve NO3-) varlığının da imidaklopridin VUV fotonlar ile sudan giderim sürecini etkilediği tespit edilmiştir. Deneysel sonuçlar imidaklopridin VUV ışıma ile arıtımını en çok etkileyen deneysel parametrenin doğal organik maddelerin yüzey sularındaki varlığından dolayı su matrisi olduğunu göstermiştir. Fakat imidaklopridin VUV ışıma ile sudan tamamen giderimi, inorganik iyonlar ve doğal organik maddelerin varlığında bile 5 dakikadan daha kısa bir sürede gerçekleşmiştir. Çözünmüş oksijenin imidaklopridin VUV foton ile bozunma ve mineralizasyon süreçleri üzerinde önemli bir etkiye sahip olmadığı tespit edilmiştir. Kinetik analizler, test edilen tüm deneysel koşullar altın imidaklopridin VUV ışıma ile gideriminin birinci derece bir reaksiyon kinetiğini izlediğini göstermiştir. Denyesel koşullara bağlı olarak imidaklopridin (Co = 5 mg/L) belirlenen bozunma hız sabitleri 1.3877 gün-1 ile 1.9213 gün-1 arasında değişiklik göstermiştir. 10 mg/L başlangıç konsantrasyonuna sahip imidaklopridin yaklaşık 80% lik mineralizasyonu 2 saat VUV ışıma sonucunda elde edilmiştir. Imidaklopridin VUV ışıma ile bozunumu sırasında bazı yan (ara) ürünlerin oluştuğu sıvı kromatografi kütle spektrometresi ile tespit edilmiştir. Bağımsız hidroliz deneyleri imidaklopridin 104 günlük hidroliz süresi boyunca asidik (pH = 3) ve doğal (orijinal, pH = 6.469) koşullar altında oldukça kararlı olup bozunmadığını göstermiştir. İmidaklopridin hidrolitik bozunması, test edilen bazik (pH = 11) koşul altında önemli ölçüde artmıştır. 0.0083 gün-1 birinci derece hidrolitik hız sabiti ve 83.51 gün yarılanma ömrü alkali çözeltide tespit edilmiştir. Ayrıca, deney bulguları VUV ışımanın tekstil boyalarının sudan arıtımında da oldukça etkili bir yöntem olduğunu göstermiştir. Kullanılan kuvars kılıfın saflığının VUV fotooksidasyon ile kirleticilerin sudan gideriminde çok önemli bir etkiye sahip olduğu da tekstil boyası deneyleriyle ortaya konulmuştur.tr_TR
dc.contributor.departmentÇevre Mühendisliğitr_TR
dc.embargo.termsAcik erisimtr_TR
dc.embargo.lift2021-10-13T08:16:49Z
dc.fundingTÜBİTAKtr_TR


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