College of Chemistry and Materials Science, Sichuan Normal University, Chengdu, 610066, China.
College of Chemistry and Materials Science, Sichuan Normal University, Chengdu, 610066, China; Key Laboratory of Treatment for Special Wastewater of Sichuan Province Higher Education System, Sichuan, Chengdu, 610066, China.
Chemosphere. 2021 Sep;278:130388. doi: 10.1016/j.chemosphere.2021.130388. Epub 2021 Mar 27.
Nitrite (NO) reduction by carbon dioxide anion radical (CO) from the activation of small molecule carboxylic acid was investigated to selectively reduce nitrite to nitrogen gas (N) However, the CO generation efficiency from the activation of small molecule carboxylic acid needs to be enhanced to increase the NO reduction efficiency. In this study, a novel and promising process for selective NO reduction was proposed based on activation of oxalic acid (OA) by UV radiation coupled with Fe. In Fe(III)/OA/UV system, the activation of OA by photo-induced electron transfer process of Fe(III)-oxalate complex and by •OH radical from the photolysis of Fe or NO could promote the generation of CO radical, which enhanced the NO reduction. The 100% removal efficiency of NO, 94.72% of total nitrogen (TN) and 94.72% of selectivity for N were achieved in Fe(III)/OA/UV/NO system, at the Fe dosage of 8 mmol/L, initial pH of 1.70, OA dosage of 16 mmol/L, initial NO concentration of 30 mg N/L, and reaction time of 180 min. CO radical played a significant role in the reduction of NO by Fe(III)/OA/UV system based on the inhibition experiments in which methyl violet was used as a quenching agent of CO radical. Based on the results from batch experiments and FTIR analysis, the activation mechanism of OA and selective reduction mechanism of NO in Fe(III)/OA/UV system was proposed.
研究了二氧化碳负离子自由基(CO)从小分子羧酸的活化中还原亚硝酸盐,以选择性地将亚硝酸盐还原为氮气(N)。然而,需要提高从小分子羧酸活化生成 CO 的效率,以提高亚硝酸盐的还原效率。在这项研究中,提出了一种基于草酸(OA)在 UV 辐射和 Fe 作用下活化的选择性还原 NO 的新工艺。在 Fe(III)/OA/UV 体系中,Fe(III)-草酸盐络合物光诱导电子转移过程和 Fe 或 NO 的光解产生的•OH 自由基对 OA 的活化可以促进 CO 自由基的生成,从而提高 NO 的还原效率。在 Fe 用量为 8 mmol/L、初始 pH 值为 1.70、OA 用量为 16 mmol/L、初始 NO 浓度为 30 mg N/L、反应时间为 180 min 的条件下,Fe(III)/OA/UV/NO 体系中 NO 的去除率达到 100%,总氮(TN)去除率为 94.72%,N 的选择性为 94.72%。基于使用甲基紫作为 CO 自由基猝灭剂的抑制实验,发现 CO 自由基在 Fe(III)/OA/UV 体系还原 NO 中起重要作用。根据批量实验和 FTIR 分析的结果,提出了 Fe(III)/OA/UV 体系中 OA 的活化机制和 NO 的选择性还原机制。