S型氧化锰/氯氧铋异质结构筑强化光催化低浓度过一硫酸盐活化降解污染物性能

doi:10.1016/S1872-2067(26)65037-1

催化学报 ›› 2026, Vol. 85: 310-321.DOI: 10.1016/S1872-2067(26)65037-1

S型氧化锰/氯氧铋异质结构筑强化光催化低浓度过一硫酸盐活化降解污染物性能

董金涛^a, 张蕊^a, 王治帅^a, 曹胜群^a, 李利娜^a, 刘高鹏^c, 王彬^a, 高艺轩^b(), 夏杰祥^a()

^a 江苏大学化学化工学院, 江苏镇江 212013
^b 中国农业科学院, 农业环境与可持续发展研究所农业清洁流域研究组, 农业农村部农业与农村生态环境重点实验室, 北京 100081
^c 海南师范大学化学与化学工程学院, 海南省电化学储能与能量转换重点实验室, 海南海口 571158

收稿日期:2025-09-04 接受日期:2025-11-01 出版日期:2026-06-18 发布日期:2026-05-18
通讯作者: *电子信箱: gaoyixuan@caas.cn (高艺轩),
xjx@ujs.edu.cn (夏杰祥).
基金资助:
国家自然科学基金(22378172);江苏省杰出青年基金(BK20240043);镇江市重点研发计划(CG2023011);国家资助博士后研究人员计划(GZC20250769)

Construction of S-scheme MnO₂/BiOCl heterojunction boosting photocatalytic low-concentration peroxymonosulfate activation for contaminants removal

Jintao Dong^a, Rui Zhang^a, Zhishuai Wang^a, Shengqun Cao^a, Lina Li^a, Gaopeng Liu^c, Bin Wang^a, Yixuan Gao^b(), Jiexiang Xia^a()

^a School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, China
^b Institute of Environment and Sustainable Development in Agriculture, Chinese Academy of Agricultural Sciences/Key Laboratory of Agricultural and Rural Eco-Environment, Ministry of Agriculture and Rural Affairs, Beijing 100081, China
^c School of Chemistry and Chemical Engineering of Hainan Normal University, Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province, Haikou 571158, Hainan, China

Received:2025-09-04 Accepted:2025-11-01 Online:2026-06-18 Published:2026-05-18
Contact: *E-mail: gaoyixuan@caas.cn (Y. Gao),
xjx@ujs.edu.cn (J. Xia).
Supported by:
National Natural Science Foundation of China(22378172);Outstanding Youth Fund of Jiangsu Province(BK20240043);Key Research and Development Program of Zhenjiang(CG2023011);Postdoctoral Fellowship Program of CPSF(GZC20250769)

摘要/Abstract

摘要：

光催化活化过一硫酸盐(PMS)是清洁高效的有机污染物降解技术, 可通过光生载流子活化PMS生成活性氧物种(ROS), 实现有机污染物高效矿化. 氯氧铋(BiOCl)材料具有毒性低、合成简便和化学稳定性高等优势, 被广泛应用于环境修复和能源转换领域. 然而, BiOCl材料的光吸收能力及载流子迁移效率低, 导致其ROS生成能力有限; 同时, BiOCl材料表面缺乏高效PMS活化位点, 导致其活化PMS产生ROS能力弱. BiOCl材料与过渡金属氧化物复合构筑异质结构, 形成高效内建电场, 促进载流子定向迁移, 提升催化材料ROS生成能力. 过渡金属氧化物表面具备丰富的PMS活化位点, 可以高效活化PMS分子, 生成大量ROS物种, 实现污染物高效去除. 作为储量丰富且可见光吸收能力强的过渡金属氧化物, 二氧化锰(MnO₂)与BiOCl材料能带位置匹配, 且具备丰富PMS活化位点, 提高ROS生成效率.

本文通过水热法合成MnO₂纳米材料, 并通过机械球磨法制备不同MnO₂含量的MnO₂/BiOCl(MOBC)光催化材料. 在可见光照射下, 以盐酸多西环素(DXC)和双酚A作为目标污染物, 评估所制备BiOCl, MnO₂及MOBC材料的光催化活化PMS降解性能. 通过引入MnO₂材料与BiOCl材料构筑异质界面, 提升内建电场强度, 形成S型电子迁移路径, 实现光生载流子定向迁移, 有效提升表面PMS活化位点数量, 强化PMS吸附活化过程, 实现ROS高效生成. 在可见光照射和低PMS浓度(0.08 mmol·L^-1)条件下, 相较于BiOCl材料, MOBC-2复合材料的DXC和BPA的氧化性能分别提升了16.3%和67.2%. 此外, MOBC-2复合材料的光催化PMS利用效率达到95.5%, 而BiOCl材料仅为36.1%. 为阐明DXC降解机理, 通过前线分子轨道与福井函数确定其易受攻击位点浓度, 为预测降解路径与中间产物提供了理论依据. 质谱分析揭示了DXC的两条主要降解路径, 涉及脱甲基, 开环及矿化反应. 此外, 毒性评估及绿豆芽培养实验证实, MOBC-2/PMS/Vis体系可显著降低DXC的生物毒性. 通过电子自旋共振波谱和自由基捕获实验分析, MOBC-2/PMS/Vis体系的ROS物种为•O₂^-, •OH, SO₄^•-和¹O₂, 其中, ¹O₂为主要活性物种. 通过密度泛函理论计算, 揭示了MnO₂/BiOCl异质结高效生成¹O₂的微观机制, 基于MnO₂的耦合效应, MnO₂/BiOCl复合材料表现出优异的PMS吸附能, 其吸附能为-3.1574 eV. 此外, 吸附氧自旋极化诱导O-O键活化, 使得自旋密度降低, 从而促进¹O₂生成. 通过自由能台阶图, 进一步分析反应动力学, 在决速步骤中, MnO₂/BiOCl异质结具有较低的吉布斯自由能变化, 有利于¹O₂生成.

综上, 通过成功构建S型氧化锰/氯氧铋异质结, 实现高效的光催化活化PMS降解污染物过程, 阐明了¹O₂高效生成机制, 为低浓度PMS的高效活化提供了新思路, 为后续高效S型异质结体系的开发和应用提供参考.

关键词: S型异质结, 光催化, 氧化锰/氯氧铋, 过一硫酸盐, 污染物降解

Abstract:

Limited by secondary pollution of PMS and active species generation capacity, the development of photocatalytic PMS activation systems should focus on the improvement of PMS utilization efficiency. In this manuscript, S-scheme MnO₂/BiOCl heterojunction were constructed for various antibiotics and endocrine disruptors removal by photocatalytic peroxymonosulfate (PMS) activation. Under visible light and the low PMS concentration (0.08 mmol·L^-1), the doxycycline hydrochloride (DXC) and bisphenol A oxidation performance of MnO₂/BiOCl-2 composites have enhanced 16.3% and 67.2% compared with that of BiOCl materials. The photocatalytic PMS utilization efficiency of MOBC-2 composites reaches to 95.5%, wherein that of BiOCl materials is 36.1%. The PMS adsorption energy of MnO₂/BiOCl composites by the density functional thoery calculation possess exceptional PMS activation ability ascribed to the coupling with MnO₂. Furthermore, the calculation of electron spin-charge density and Gibbs free energy change demonstrates MnO₂/BiOCl composites can react with PMS for ¹O₂ formation. The liquid chromatography-tandem mass spectrometry measurement and Fukui function has been employed for inferring the intermediates of DXC in PMS oxidation process. This manuscript provides research insights and scientific references for construction of S-scheme heterojunction to employ in visible-light-driven low-concentration PMS activation process.

Key words: S-scheme heterojunction, Photocatalysis, MnO₂/BiOCl, Peroxymonosulfate, Pollutants removal

董金涛, 张蕊, 王治帅, 曹胜群, 李利娜, 刘高鹏, 王彬, 高艺轩, 夏杰祥. S型氧化锰/氯氧铋异质结构筑强化光催化低浓度过一硫酸盐活化降解污染物性能[J]. 催化学报, 2026, 85: 310-321.

Jintao Dong, Rui Zhang, Zhishuai Wang, Shengqun Cao, Lina Li, Gaopeng Liu, Bin Wang, Yixuan Gao, Jiexiang Xia. Construction of S-scheme MnO₂/BiOCl heterojunction boosting photocatalytic low-concentration peroxymonosulfate activation for contaminants removal[J]. Chinese Journal of Catalysis, 2026, 85: 310-321.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65037-1

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Fig. 1. (a) The schematic illustration for preparation process of MOBC-2 composites. The XPS spectra of MnO2, BiOCl and MOBC-2 composites: Bi 4f (b), Mn 2p (c), Cl 2p (d), and O 1s (e). (f) The electrostatic potential calculation of BiOCl materials and MnO2 materials.

Fig. 2. SEM images of BiOCl materials (a), MnO2 materials (d) and MOBC-2 composites (g). TEM images of BiOCl materials (b,c), MnO2 materials (e,f) and MOBC-2 composites (h,i). (j) TEM images and the corresponding elemental mapping images of MOBC-2 composites.

Fig. 3. The DXC degradation activity of MnO2, BiOCl and MOBC-x composites (a), and MOBC-2 composites with different PMS concentrations (b). The DXC degradation activity of MOBC-2/PMS/Vis system under cation interference (c) and anion interference condition (d). (e) The cycle stability of MOBC-2 composites for DXC removal. (f) The different pollutant degradation performance of MOBC-2 composites. (g) The BPA degradation activity of BiOCl and MOBC-2 composites. The UV-vis absorption spectra of iodometric PMS measure-ment systems of BiOCl (h) and MOBC-2 composites (i). Reaction conditions: [catalysts] = 0.2 g·L-1, [PMS] = 0.08 mmol·L-1, [pollutants] = 10 mg·L-1.

Fig. 4. (a) UV-vis DRS spectra of MnO2, BiOCl and MOBC-x composites. The transient photocurrents response (b), EIS spectra (c), PL spectra (d), and LSV curves (e,f) of BiOCl and MOBC-2 composites under different conditions.

Fig. 5. ESR spectra of DMPO-•O2− (a), DMPO-•OH and DMPO-SO4•-(b), and TEMPO-1O2 (c) in various systems. (d) The •O2−, 1O2, •OH and SO4•− species capture measurements of MOBC-2/PMS/Vis system.

Fig. 6. (a) The energy band diagram of MOBC composites before and after contact; charge transfer pathway of MOBC composites. (b) The possible photocatalytic PMS degradation mechanism in MOBC-2 composites.

Fig. 7. (a) The optimized molecule structure of DXC molecules. (b) HOMO and LUMO of DXC molecules. (c) The distribution of orbit weight Fukui function on the plane. (d) The orbital weights of f+, f−, f0. (e) The DXC possible degradation pathways for MOBC-2/PMS/Vis systems.

Fig. 8. Mechanism analysis of 1O2 generation of BiOCl, MnO2 and MnO2/BiOCl materials. (a) The schematic energy band diagrams showing charge transfer pathway for MnO2/BiOCl materials. (b) Gibbs free energy diagram of various intermediates at different adsorption sites in PMS. (c) pDOS diagram of oxygen, (d-f) the electron configuration in oxygen and 1O2. (g) The spin electron density of adsorbed oxygen and O-O (SO5). (h) The adsorption energy and rate-determining step energy changes.

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S型氧化锰/氯氧铋异质结构筑强化光催化低浓度过一硫酸盐活化降解污染物性能

Construction of S-scheme MnO₂/BiOCl heterojunction boosting photocatalytic low-concentration peroxymonosulfate activation for contaminants removal

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S型氧化锰/氯氧铋异质结构筑强化光催化低浓度过一硫酸盐活化降解污染物性能

Construction of S-scheme MnO2/BiOCl heterojunction boosting photocatalytic low-concentration peroxymonosulfate activation for contaminants removal

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Construction of S-scheme MnO₂/BiOCl heterojunction boosting photocatalytic low-concentration peroxymonosulfate activation for contaminants removal