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臭氧工艺中两种典型 N-杂环化合物的降解特性:效能、动力学、途径、毒性及其在实际生物预处理煤气化废水中的应用。

Degradation characteristics of two typical N-heterocycles in ozone process: Efficacy, kinetics, pathways, toxicity and its application to real biologically pretreated coal gasification wastewater.

机构信息

State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin, 150090, China.

School of Engineering, South China Agriculture University, Guangzhou, 510642, China.

出版信息

Chemosphere. 2018 Oct;209:319-327. doi: 10.1016/j.chemosphere.2018.06.067. Epub 2018 Jun 14.

Abstract

Ozonation of pyridine and indole was investigated both in aqueous solution and biologically pretreated coal gasification wastewater (BPCGW). Experimental results showed that the removal of indole was hardly affected by pH value. Direct reaction rate constant of ozone with pyridine increased from 0.18 M s (protonated pyridine) to 3.03 M s (molecular pyridine), and that with molecular indole was 8.6 × 10 M s. Seven and five transformation intermediates were observed for pyridine and indole, respectively. Ozonation pathways were proposed as hydroxylation, opening and cleavage of the aromatic ring. It was found that ammonia nitrogen (NHN) increased by 3.3 mg L in ozone process, suggesting the broken of the CN bonds of pyridine, indole and other N-heterocyclic compounds. In terms of biochemical oxygen demand to chemical oxygen demand (BOD/COD), toxicity and resazurin dehydrogenase activity (DHA), the biodegradability was improved after ozone treatment, indicating the possibility of ozone combined with biosystem for the treatment of BPCGW. The results of gas chromatograph and mass spectrometry (GC-MS) indicated that primary products during first 10 min might lead to the obstinate toxicity, which was further proved by US Environmental Protection Agency (US-EPA) test. This study would assist in obtaining a better understanding of the application of ozonation pretreatment in BPCGW.

摘要

臭氧氧化吡啶和吲哚的研究分别在水溶液中和生物预处理煤气化废水中(BPCGW)进行。实验结果表明,吲哚的去除几乎不受 pH 值的影响。臭氧与吡啶的直接反应速率常数从 0.18 M/s(质子化吡啶)增加到 3.03 M/s(分子吡啶),而与分子吲哚的反应速率常数为 8.6×10 M/s。分别观察到吡啶和吲哚的 7 种和 5 种转化中间产物。提出了臭氧氧化的途径为羟化、开环和芳环断裂。研究发现,臭氧过程中氨氮(NHN)增加了 3.3mg/L,表明吡啶、吲哚和其他含氮杂环化合物中的 CN 键断裂。就生化需氧量与化学需氧量之比(BOD/COD)、毒性和 Resazurin 脱氢酶活性(DHA)而言,臭氧处理后可提高生物降解性,表明臭氧与生物系统联合处理 BPCGW 的可能性。气相色谱和质谱(GC-MS)的结果表明,前 10 分钟的主要产物可能导致顽固毒性,这进一步被美国环保署(US-EPA)的测试所证实。本研究将有助于更好地了解臭氧预处理在 BPCGW 中的应用。

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