本文選題：磷酸銀基復(fù)合催化劑　切入點(diǎn)：阿特拉津　出處：《華中農(nóng)業(yè)大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：阿特拉津(Atrazine)作為一種在世界范圍內(nèi)廣泛使用的除草劑,能夠有效防治農(nóng)田雜草生長(zhǎng)以提高農(nóng)業(yè)生產(chǎn)效益,但是殘留的阿特拉津能進(jìn)入土壤、河流、湖泊,對(duì)地下水、地表水造成污染,并隨著生物鏈的富集,對(duì)植物、動(dòng)物、人類造成不同程度的危害。近年來(lái),隨著光催化技術(shù)的不斷發(fā)展,簡(jiǎn)單、廉價(jià)、高效地光催化降解阿特拉津成為人們研究的熱點(diǎn)。Ag_3PO_4作為一種新型高活性可見光催化劑,已在光解制氧、還原CO_2、降解NO_x化合物、降解有機(jī)污染物等方面開展了廣泛研究,但對(duì)其光催化降解阿特拉津的研究較少。本文利用不同改性方法制備了磷酸銀基復(fù)合催化劑(Au NRs/Ag_3PO_4、Mo-Ag_3PO_4)。通過SEM、XRD、XPS等一系列手段進(jìn)行表征,檢測(cè)了其物理和化學(xué)結(jié)構(gòu)性質(zhì)。研究了可見光照射下,磷酸銀基復(fù)合催化劑(Au NRs/Ag_3PO_4、Mo-Ag_3PO_4)光催化降解水中阿特拉津的降解效果。磷酸銀基復(fù)合催化劑光催化降解阿特拉津的研究表明,當(dāng)反應(yīng)體系初始pH=6時(shí),其光催化活性最好,并且隨著光催化過程的進(jìn)行,體系的pH值逐漸降低。通過自由基捕獲實(shí)驗(yàn)發(fā)現(xiàn),催化反應(yīng)過程中主要的活性物種為h~+和·OH自由基。利用高效液相色譜-質(zhì)譜(LC-MS)、離子色譜(IC)測(cè)定了復(fù)合催化劑光催化降解阿特拉津的中間產(chǎn)物:2-羥基-4-乙胺基-6-異丙胺基-1,3,5-三嗪、2-氯-4-氨基-6-異丙胺基-1,3,5-三嗪、2-羥基-4-氨基-6-異丙胺基-1,3,5-三嗪、2,4-二羥基-6-異丙胺基-1,3,5-三嗪等,并推測(cè)出磷酸銀基復(fù)合催化劑催化降解阿特拉津的可能機(jī)理:在可見光的照射下,Ag_3PO_4受光激發(fā)產(chǎn)生光生e~-與h~+,復(fù)合體系中Au NRs以及Mo元素的存在有利于促進(jìn)e~-的轉(zhuǎn)移,提高催化活性;光生h+則與反應(yīng)體系中的H2O反應(yīng)生成·OH和H~+,使體系的pH值隨著反應(yīng)的進(jìn)行而降低;與此同時(shí),產(chǎn)生的·OH自由基分別進(jìn)攻阿特拉津分子的C-Cl鍵、側(cè)鏈乙胺基仲碳原子及側(cè)鏈異丙胺基中心碳原子,經(jīng)脫氯-羥基化和脫烷基作用等一系列的化學(xué)反應(yīng),得到最后的產(chǎn)物為三聚氰酸,三聚氰酸會(huì)被進(jìn)一步礦化成H_2O、CO_2、NO_3~-。本論文不僅豐富了磷酸銀基復(fù)合催化劑在光催化降解農(nóng)藥有機(jī)污染領(lǐng)域的應(yīng)用,而且為光催化降解阿特拉津的實(shí)際應(yīng)用提供了理論基礎(chǔ)。
[Abstract]:Atrazine (Atrazine), a herbicide that is widely used around the world, can effectively control the growth of weeds in farmland to improve agricultural productivity, but the residual atrazine can enter the soil, rivers, lakes, and groundwater. Surface water causes pollution, and with the enrichment of biological chain, it causes varying degrees of harm to plants, animals and human beings. In recent years, with the continuous development of photocatalytic technology, simple, cheap, High efficient photocatalytic degradation of atrazine has become a hot topic. Ag3PO4, as a new type of highly active visible light catalyst, has been widely studied in photodegradation of oxygen, reduction of CO _ 2, degradation of NO_x compounds, degradation of organic pollutants, and so on. However, the photocatalytic degradation of atrazine was seldom studied. In this paper, silver phosphate-based composite catalyst au NRsr / AgS / AW / AW / APS / AW / AW / Ag / 3PO4 / M were prepared and characterized by a series of methods, such as SEM- XRD- XPS, Mo-AgSP, 3PO4, and so on. The physical and chemical properties of Atrazine were investigated. The photocatalytic degradation of atrazine in water was studied by using silver phosphate based composite catalyst au NRs / Ag3PO4 / Snap4Mo-Ag3PO4 under visible light irradiation. The photocatalytic degradation of atrazine by silver phosphate-based composite catalyst was studied. When the initial pH of the reaction system was 6:00, the photocatalytic activity of the system was the best, and the pH value of the system gradually decreased with the process of photocatalysis. H ~ and 路OH radicals were the main active species in the catalytic reaction. The intermediate product of atrazine was determined by high performance liquid chromatography-mass spectrometry (HPLC-MS) and ion chromatography (ICIC). 2-chloro-4-amino-6-isopropylamino-2-hydroxy-4-amino-6-isopropylamino-2-hydroxy-4-amino-6-isopropylaminyl -1-triazine, 2-hydroxy-4-amino-6-isopropylamino-2-triazine, 5-triazino-5-triazino-2-dihydroxy-6-isopropylamine, etc., The possible mechanism of the degradation of atrazine by silver phosphate based composite catalyst was inferred: Ag3PO4 was stimulated by visible light to produce photogenerated edo- and h-, and the presence of au NRs and Mo in the composite system was helpful to promote the transfer of ego-. The photogenerated h reacts with H 2O in the reaction system to form 路OH and H ~, which makes the pH value of the system decrease with the reaction. At the same time, the generated 路OH free radicals attack the C-Cl bond of atrazine molecule respectively. After a series of chemical reactions, such as dechlorination, hydroxylation and dealkylation, the final product of the secondary carbon atom and the central carbon atom of isopropylamine group in the side chain was obtained by a series of chemical reactions such as dechlorination, hydroxylation and dealkylation. Tripolycyanoic acid will be further mineralized to form S / C _ 2O _ 2 CO _ 2O _ 3C _ 3. This paper not only enriches the application of silver phosphate based composite catalyst in the field of photocatalytic degradation of pesticide organic pollution, but also provides a theoretical basis for the practical application of photocatalytic degradation of atrazine.
【學(xué)位授予單位】：華中農(nóng)業(yè)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：X592;O643.36;O644.1

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