本文選題：腐殖化 + 阿特拉津��； 參考：《南京農(nóng)業(yè)大學(xué)》2015年碩士論文

【摘要】：腐殖化是外源有機物在環(huán)境中轉(zhuǎn)化的一個重要途徑,它導(dǎo)致小分子物質(zhì)聚合或與土壤有機質(zhì)結(jié)合,最終形成無定型的土壤有機質(zhì)。全面了解腐殖化過程中有機污染物轉(zhuǎn)化的機理,可為科學(xué)評估腐殖化過程對有機污染物在環(huán)境中的轉(zhuǎn)化和風(fēng)險提供可靠依據(jù)。本研究選擇阿特拉津(ATZ)作為研究對象,對ATZ與有機質(zhì)結(jié)合的機理進行深入探究,分析產(chǎn)物。研究結(jié)果表明,在一系列結(jié)構(gòu)不同的腐殖質(zhì)模擬化合物中,苯胺明顯促進ATZ的去除。由于ATZ中含有的C1原子具有強電負(fù)性,使得與之相連的碳原子很容易受到苯胺結(jié)構(gòu)中親核基團(-NH2)的攻擊,因此這兩種物質(zhì)間可能通過親核取代途徑進行結(jié)合。本研究還選取環(huán)境中普遍存在的氨基酸/多肽等親核物質(zhì)對ATZ形成結(jié)合態(tài)殘留的影響進行研究。實驗結(jié)果表明,含巰基(-SH)的氨基酸/多膚可有效地去除ATZ,氨基酸/多肽中與ATZ反應(yīng)的活性官能團是-SH。除含硫氨基酸/多肽外,硫醇和硫化鈉也能夠與ATZ反應(yīng)。本研究選取鹵代酚作為典型的酚類有機污染物,探究其在漆酶催化過程中的反應(yīng)動力學(xué),探討了腐植酸(HA)、金屬離子對鹵代酚轉(zhuǎn)化的影響,深入分析反應(yīng)產(chǎn)物。實驗結(jié)果表明,漆酶催化氧化鹵代酚遵循二級反應(yīng)動力學(xué)規(guī)律。HA存在時,抑制鹵代酚的轉(zhuǎn)化,反應(yīng)遵循一級反應(yīng)動力學(xué)規(guī)律;通過動力學(xué)模型分析HA的作用機理,結(jié)果表明HA充當(dāng)鹵代酚自由基的淬滅劑。1 mmol·L-1 Cu2+促進鹵代酚的轉(zhuǎn)化,隨Cu2+濃度增加則會抑制鹵代酚的轉(zhuǎn)化。鹵代酚自由基通過C-C或C-O共價鍵結(jié)合分別生成羥基鹵代聯(lián)苯和羥基鹵代聯(lián)苯醚等聚合產(chǎn)物。部分聚鹵代產(chǎn)物具有內(nèi)分泌干擾性,對生態(tài)系統(tǒng)和人類健康存在一定威脅。本研究為聚鹵代芳香族化合物的來源提供了科學(xué)依據(jù)。此外,利用模型化合物(3,5-二羥基苯甲酸、間苯二酚)模擬腐殖質(zhì)對鹵代酚反應(yīng)的影響。結(jié)果表明,3,5-二羥基苯甲酸一定程度上模擬了 HA的反應(yīng),間苯二酚可抑制鹵代酚的轉(zhuǎn)化,但隨其投加量的增加,抑制效果沒有顯著變化。反應(yīng)過程中有鹵代酚與模型化合物通過C-C/C-O交叉聚合的產(chǎn)物和具有二VA英結(jié)構(gòu)的物質(zhì)生成。
[Abstract]:Humification is an important way for the transformation of exogenous organic matter in the environment, which leads to the aggregation of small molecular matter or the combination with soil organic matter, resulting in the formation of amorphous soil organic matter. An overall understanding of the mechanism of organic pollutant transformation during humification can provide a reliable basis for the scientific assessment of the transformation and risk of organic pollutants in the environment. In this study, atrazine (ATZ) was selected as the research object, and the mechanism of the combination of ATZ and organic matter was studied in depth, and the product was analyzed. The results showed that aniline promoted the removal of ATZ in a series of humus mimic compounds with different structures. Due to the strong electronegativity of C1 atoms in ATZ, the associated carbon atoms are vulnerable to attack by the nucleophilic group (-NH _ 2) in aniline structure, so the two substances may be bound by nucleophilic substitution. The effect of nucleophilic substances such as amino acid / polypeptide on the formation of binding residues of ATZ was also studied. The results showed that the amino acid / polypeptide containing sulfhydryl group could effectively remove ATZs, and the active functional group which reacted with ATZ in amino acid / polypeptide was -SHH. Mercaptan and sodium sulfide can react with ATZ in addition to amino acid / polypeptide containing sulfur. In this study, halogenated phenols were selected as typical phenolic organic pollutants, and their reaction kinetics in laccase catalysis was studied. The effects of humic acid and metal ions on the conversion of halogenated phenols were discussed, and the reaction products were analyzed in depth. The results showed that laccase catalyzed oxidation of halogenated phenol followed the second order reaction kinetics law. In the presence of HA, the transformation of halogenated phenol was inhibited, and the reaction followed the first order reaction kinetics law, and the mechanism of HA action was analyzed by kinetic model. The results show that HA acts as the quenching agent of halogenated phenol radical. 1 mmol L-1 Cu2 can promote the transformation of halogenated phenol. With the increase of Cu2 concentration, the transformation of halogenated phenol is inhibited. Hydroxyl halogenated biphenyls and hydroxy halogenated diphenyl ethers were synthesized from halogenated phenols by C-C or C-O covalent bonding respectively. Some polyhalogenated products are endocrine disrupting, which is a threat to ecosystem and human health. This study provides a scientific basis for the origin of polyhalogenated aromatic compounds. In addition, the effects of humus on the reaction of halogenated phenols were simulated by using the model compounds of 3 ~ (3) -dihydroxybenzoic acid and resorcinol. The results showed that the HA reaction was simulated to a certain extent, and resorcinol could inhibit the transformation of halogenated phenol, but with the increase of its dosage, the inhibitory effect did not change significantly. During the reaction, halogenated phenols and model compounds were synthesized by C-C/C-O cross-polymerization and diVA structure.
【學(xué)位授予單位】：南京農(nóng)業(yè)大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X132

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