环境化学2024,Vol.43Issue(12) :4228-4237.DOI:10.7524/j.issn.0254-6108.2023062102

醇对喹啉超临界水氧化的强化降解作用

Enhanced degradation of quinoline with alcohols in supercritical water oxidation

张洁 田欣悦 李博文 黄荣普 孟海鱼 郑小波
环境化学2024,Vol.43Issue(12) :4228-4237.DOI:10.7524/j.issn.0254-6108.2023062102

醇对喹啉超临界水氧化的强化降解作用

Enhanced degradation of quinoline with alcohols in supercritical water oxidation

张洁 1田欣悦 2李博文 2黄荣普 2孟海鱼 2郑小波2
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作者信息

  • 1. 交通新能源开发、应用与汽车节能陕西省重点实验室,长安大学,西安,710064
  • 2. 西北旱区生态水利国家重点实验室,西安理工大学,西安,710048
  • 折叠

摘要

对工业废水与污泥中含氮污染物的高效处理已成为一项重要的环境问题.本研究以典型含氮化合物喹啉为研究对象,探索醇(甲醇、乙二醇和丙三醇)对喹啉超临界水氧化(SCWO)的强化降解机制,获得了反应参数对喹啉中碳、氮元素降解的影响规律,并且对喹啉的SCWO反应路径进行分析.研究结果表明,在压力25 MPa、氧化系数1.5、反应温度450 ℃时,添加800 mmol L-1甲醇,可使1.125%wt喹啉SCWO反应的XTOC和 XTN分别达到95.9%和62.7%,比纯喹啉反应的71.6%和56.2%高得多.提高反应温度和氧化系数可改善甲醇的动力学效应.另外,对甲醇、乙二醇和丙三醇的强化降解效果进行对比得出,由于多元醇优异的动力学与热效应,三者对喹啉氧化的促进作用顺序为CH3OH<(CH2OH)2<C3H8O3.喹啉的SCWO降解起始于吡啶环开环,发生羟基化、断键、开环等过程.

Abstract

Effective treatment of nitrogen-containing pollutants in industrial wastewater and sludge has become an important environmental issue.The typical nitrogen-containing compound quinoline was employed to explore the enhanced degradation effects of active alcohols(methanol,ethylene glycol,and glycerol)during supercritical water oxidation(SCWO)of quinoline.The influences of reaction parameters on degradation of carbon and nitrogen in quinoline were studied.The SCWO reaction path of quinoline was analyzed.The results show that the XTOC and XTN for SCWO of 1.125%wt quinoline with 800 mmol·L-1 methanol were,respectively,95.9%and 62.7%at pressure of 25 MPa,oxidation coefficient of 1.5,and reaction temperature of 450 ℃,whereas only 71.6%and 56.2%were attained in the pure quinoline reaction.Increasing the reaction temperature and oxidation coefficient can improve the kinetic effect of methanol.In addition,the comparison of the enhanced degradation effects of methanol,ethylene glycol,and glycerol indicates that,due to the superior kinetic and thermal effects of polyols,the order of three alcohols'promotion effects on quinoline oxidation was CH3OH<(CH2OH)2<C3H8O3.Finally,SCWO of quinoline was initiated by ring opening of the pyridine ring,and conducted hydroxylation,bond breaking and ring opening reactions.

关键词

超临界水/喹啉//氧化

Key words

supercritical water/quinoline/alcohol/oxidation

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出版年

2024
环境化学
中国科学院生态环境研究中心

环境化学

CSTPCDCSCD北大核心
影响因子:1.049
ISSN:0254-6108
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