Concentrated-degradation “reactor” for in-situ tetrabromobisphenol A removal based on the precise design of pollution/photocatalyst micro-interface

IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2025-04-08 DOI:10.1016/j.seppur.2025.132939
Silong Wang , Zesen Shang , Jin Xu , Li Xiong , Chengzhuo Yu , Fanglan Geng , Huasheng Wu , Jitao Lv , Lixia Zhao , Yawei Wang , Guibin Jiang
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Abstract

Concentration-degradation is an effective strategy for removing emerging pollutants at low concentrations, yet the design of the contaminant/catalyst micro-interface remains a challenge. In this work, tetrabromobisphenol A (TBBPA) as a model pollutant, a precise micro-interface based on ZrO2/ZnIn2S4 hollow microspheres were designed to construct a concentration-degradation “reactor” for removing low concentrations of pollutants in water. The ZrO2/ZnIn2S4 achieved efficient photocatalytic degradation (92.95 %) of TBBPA with excellent adsorption capacity (289.05 mg g−1). The experimental results and DFT calculation indicated that a surface electric field was developed with special interfacial interactions of hydroxyl/Zr and Br/S vacancies, which facilitated the attack of h+ on the TBBPA to achieve rapid separation of photogenerated carriers. In the presence of e-, h+, ·OH, and ·O2, the TBBPA was converted to small molecules by debromination, hydroxyl substitution, and beta-scission pathways. This work provides novel insights into the adsorption and degradation of pollutants from an interfacial perspective and presents the potential solution for the removal of trace emerging pollutants.

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基于污染/光触媒微界面精确设计的原位四溴双酚A浓缩降解“反应器
浓度降解是去除低浓度新兴污染物的有效策略,但污染物/催化剂微界面的设计仍是一项挑战。本研究以四溴双酚 A(TBBPA)为模型污染物,设计了一种基于 ZrO2/ZnIn2S4 空心微球的精确微界面,构建了一个浓度降解 "反应器",用于去除水中的低浓度污染物。ZrO2/ZnIn2S4 实现了对四溴双酚 A 的高效光催化降解(92.95%),并具有优异的吸附能力(289.05 mg g-1)。实验结果和 DFT 计算表明,羟基/Zr 和 Br/S 空位的特殊界面相互作用形成了表面电场,促进了 h+ 对 TBBPA 的攻击,实现了光生载流子的快速分离。在 e-、h+、-OH 和 -O2- 的存在下,TBBPA 通过脱溴、羟基取代和β-分裂途径转化为小分子。这项工作从界面角度为污染物的吸附和降解提供了新的见解,并为去除痕量新兴污染物提供了潜在的解决方案。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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