纳米级顺序反应器设计在催化臭氧处理中有效去除消毒副产物前体

IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL 环境科学与技术 Pub Date : 2024-07-02 DOI:10.1021/acs.est.3c09295
Zilong Song, Jiaguang Xu, Jingmeng Guan, Peng Wang, Junlang Qiu, Yu Lei, Xinran Zhang, Qingqing Kong, Yangjian Zhou, Xin Yang
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引用次数: 0

摘要

在水处理过程中,转化溶解有机物(DOM)是减少消毒副产物(DBP)形成的重要方法。虽然催化臭氧可以有效转化 DOM,但由于 DOM 转化过程中醛、酮和硝基化合物中间产物的积累,DBP 的形成潜力往往会增加。在本研究中,我们提出了一种新型 DOM 顺序氧化策略,可有效降低这些中间产物的累积水平。这是通过开发一种具有定制表面和纳米封闭活性位点的催化臭氧催化剂来实现的。该催化剂具有独特的封闭结构,其中 Mn-N4 分子均匀地固定在催化剂表面和纳米孔(5-20 Å)内。这种设计使催化剂表面的大分子量 DOM 得到降解,而转化后的小分子量 DOM 则进入纳米孔,并在封闭效应的作用下迅速降解。要有效减少这些臭氧难降解中间产物,就必须生成作为主要反应物的*Oad。这使得碳质和氮质 DBP 前体以及溴化 DBP 前体的去除率超过 70%。这项研究强调了纳米级顺序反应器设计的重要性,并为通过催化臭氧过程消除 DBP 前体提供了新的见解。
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Nanoscale Sequential Reactor Design Achieves Effective Removal of Disinfection Byproduct Precursors in Catalytic Ozonation.

Transforming dissolved organic matter (DOM) is a crucial approach to alleviating the formation of disinfection byproducts (DBPs) in water treatment. Although catalytic ozonation effectively transforms DOM, increases in DBP formation potential are often observed due to the accumulation of aldehydes, ketones, and nitro compound intermediates during DOM transformation. In this study, we propose a novel strategy for the sequential oxidation of DOM, effectively reducing the levels of accumulation of these intermediates. This is achieved through the development of a catalyst with a tailored surface and nanoconfined active sites for catalytic ozonation. The catalyst features a unique confinement structure, wherein Mn-N4 moieties are uniformly anchored on the catalyst surface and within nanopores (5-20 Å). This design enables the degradation of the large molecular weight fraction of DOM on the catalyst surface, while the transformed smaller molecular weight fraction enters the nanopores and undergoes rapid degradation due to the confinement effect. The generation of *Oad as the dominant reactive species is essential for effectively reducing these ozone refractory intermediates. This resulted in over 70% removal of carbonaceous and nitrogenous DBP precursors as well as brominated DBP precursors. This study highlights the importance of the nanoscale sequential reactor design and provides new insights into eliminating DBP precursors by the catalytic ozonation process.

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来源期刊
环境科学与技术
环境科学与技术 环境科学-工程:环境
CiteScore
17.50
自引率
9.60%
发文量
12359
审稿时长
2.8 months
期刊介绍: Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences. Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.
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