金属硼化物作为增强持久类芬顿反应的优良助催化剂:金属和硼的双共催化中心

IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Shuang Meng, Minglu Sun, Peng Zhang, Chenying Zhou, Chuanshu He, Heng Zhang, Yang Liu, Zhaokun Xiong, Peng Zhou* and Bo Lai*, 
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引用次数: 1

摘要

在铁基深度氧化工艺(AOPs)中,氧化分解诱导的活性氧(ROS)生成的持续电子供应是长期存在的微污染物氧化的主要贡献者。本文中,具有双活性位点和优异导电性的金属硼化物作为一类新型助催化剂,通过稳定地向非活性Fe(III)提供电子,可以有效克服类芬顿反应固有的缺点。在金属硼化物中,硼化钨(WB)表现出显著的共催化性能,领先于常见的非均相共催化剂,并且具有极高的稳定性。定性和半定量试验表明,在WB/Fe(III)/PDS体系中均产生羟基自由基、硫酸盐自由基和铁(IV)-氧络合物,Fe(IV)诱导的甲基苯基亚砜分解率高达72%。此外,ROS的产生效率以及自由基和非自由基途径的相对比例随着不同的实验条件(PDS、WB和溶液pH的剂量)和水基质而变化。由于暴露的金属活性位点与具有WB还原性的非金属硼之间的协同作用,大大加快了Fe(II)再生的速率决定步骤。此外,表面氧化钨和氧化硼的自溶解导致表面更新,从而在长期运行中可持续地减少铁(III)。我们的发现为增强AOPs用于水修复领域提供了一种有效和可持续的策略。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Metal Borides as Excellent Co-Catalysts for Boosted and Long-Lasting Fenton-like Reaction: Dual Co-Catalytic Centers of Metal and Boron

Metal Borides as Excellent Co-Catalysts for Boosted and Long-Lasting Fenton-like Reaction: Dual Co-Catalytic Centers of Metal and Boron

The continuous electron supply for oxidant decomposition-induced reactive oxygen species (ROS) generation is the main contributor for the long-standing micropollutant oxidation in the iron-based advanced oxidation processes (AOPs). Herein, as a new class of co-catalysts, metal borides with dual active sites and preeminent conductive performance can effectively overcome the inherent drawback of Fenton-like reactions by steadily donating electrons to inactive Fe(III). Among the metal borides, tungsten boride (WB) exhibits a significant co-catalytic performance run ahead of common heterogeneous co-catalysts and exceptionally high stability. Based on qualitative and semi-quantitative tests, the hydroxyl radical, sulfate radical, and iron(IV)-oxo complex are all produced in the WB/Fe(III)/PDS system and Fe(IV)-induced methyl phenyl sulfoxide decomposition is up to 72%. Moreover, the production efficiency of ROS and relative proportions of radical and nonradical pathways change with various experimental conditions (dosages of PDS, WB, and solution pH) and water matrices. The rate-determining step of Fe(II) regeneration is greatly accelerated resulting from the synergetic effect between exposed metallic reactive sites and nonmetallic boron with reductive properties of WB. In addition, the self-dissolution of surface tungsten oxide and boron oxide leads to a renovated surface for sustainable Fe(III) reduction in long-term operations. Our discovery provides an efficient and sustainable strategy in the field of enhanced AOPs for water remediation.

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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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