Simultaneous degradation of organoarsenic and immobilization of arsenate by an electroactive CuFe2O4-CNT/peroxymonosulfate platform: Insights into the distinct roles of the Cu and Fe sites

IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Journal of Hazardous Materials Pub Date : 2025-03-15 Epub Date: 2024-12-20 DOI:10.1016/j.jhazmat.2024.136952
Xin Gao , Wenxiang Li , Yanbiao Liu , Hao Sun , Haitao Wang , Yi Wang
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Abstract

Phenylarsonic acid (PAA) compounds, widely used in animal husbandry, pose a considerable environmental threat owing to their potential transformation into toxic inorganic arsenic species. To efficiently decontaminate PAA and adsorb secondary As(V), a hybrid CuFe2O4-modified carbon nanotube (CuFe2O4-CNT) filter was developed in this study. The hybrid CuFe2O4-CNT filter functioned as an effective catalyst, convective filtration medium, electrode, and adsorbent. Moreover, it removed 97 % PAA within 80 min in circulation mode under optimal conditions (25 °C, pH0 = 7, peroxymonosulfate [PMS] = 1.5 mM, and voltage = 1.0 V), with a total As removal efficiency of 94 %. Experimental and theoretical studies showed that the (100) and (211) planes of CuFe2O4-CNT contributed to PMS activation and As(V) adsorption, respectively. Quantum chemical calculations and high-performance liquid chromatography-mass spectrometry analysis determined the energy barriers for reactions between the transient state and SO4•− and HO, based on which potential PAA degradation pathways were proposed. Additionally, the negligible loss of efficiency in practical water samples and acceptable leached metal ion concentrations (Cu < 0.1 mg/L and Fe < 0.15 mg/L) confirmed the reusability and stability of the filter. This study provides a promising strategy for organoarsenic decontamination by combining electrocatalytic PMS oxidation and filtration techniques.

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电活性CuFe2O4-CNT/过氧单硫酸盐平台同时降解有机砷和固定化砷酸盐:Cu和Fe位点的不同作用的见解
苯拉森酸(PAA)化合物广泛应用于畜牧业,由于其可能转化为有毒的无机砷,对环境造成了相当大的威胁。为了高效去除PAA和吸附次生As(V),研究了cufe2o4修饰碳纳米管(CuFe2O4-CNT)混合过滤器。CuFe2O4-CNT杂化过滤器作为有效的催化剂、对流过滤介质、电极和吸附剂。此外,在最佳条件(25°C, pH0 = 7,过氧单硫酸盐[PMS] = 1.5 mM,电压= 1.0 V)下,循环模式下80 min内去除97%的PAA,总As去除率为94%。实验和理论研究表明,CuFe2O4-CNT的(100)面和(211)面分别对PMS活化和As(V)吸附有贡献。量子化学计算和高效液相色谱-质谱分析确定了瞬态与SO4•−和HO•之间反应的能垒,并在此基础上提出了PAA的潜在降解途径。此外,在实际水样和可接受的浸出金属离子浓度(Cu <;0.1 mg/L和Fe <;0.15 mg/L),证实了过滤器的可重复使用性和稳定性。本研究提供了一种结合电催化PMS氧化和过滤技术的有机砷净化策略。
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来源期刊
Journal of Hazardous Materials
Journal of Hazardous Materials 工程技术-工程:环境
CiteScore
25.40
自引率
5.90%
发文量
3059
审稿时长
58 days
期刊介绍: The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.
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