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用于过一硫酸盐活化的具有双S型异质结的MoS@MoO/(Cu/g-CN)三元复合材料的合成及其可见光照射性能

Synthesis of MoS@MoO/(Cu/g-CN) ternary composites with double S-scheme heterojunction for peroxymonosulfate activation exposing to visible light.

作者信息

Hong Chuangbin, Wang Wenguang, Wu Liangpeng, Zhou Jiehang, Long Shimin, Zhou Wentao, Guo Yuxi

机构信息

School of Materials and Energy, Guangdong University of Technology, Guangzhou Higher Education Mega Center 100#, Guangzhou 510006, PR China.

School of Materials and Energy, Guangdong University of Technology, Guangzhou Higher Education Mega Center 100#, Guangzhou 510006, PR China.

出版信息

J Colloid Interface Sci. 2025 Jan 15;678(Pt B):639-656. doi: 10.1016/j.jcis.2024.09.076. Epub 2024 Sep 11.

Abstract

The construction of semiconductor heterojunction is an effective way for charge separation in photocatalytic degradation of pollutants. In this study, a novel MoS@MoO/(Cu/g-CN) ternary composites (MMCCN) was prepared via a simple calcination method. The as-prepared composites exhibited exceptional performance in activating peroxymonosulfate (PMS) for the degradation of rhodamine B (RhB). The activity testing results indicated that 99.41 % of RhB (10 mg·L, 10 mL) was effectively removed by the synergistic effect of composites photocatalyst (0.1 g·L) and PMS (0.1 g·L) under visible light irradiation for 40 min. Its reaction rate constant exceeded that of Cu/g-CN, MoO and MoS by a factor of 3.56, 17.30 and 11.73 times, respectively. The crystal structure, band gap and density of states (DOS) of the semiconductors were calculated according to the density functional theory (DFT). Free radical trapping tests and electron spin resonance spectroscopy validated that O, O and h are primary reactive species participating in the decomposition of RhB. The ternary composites demonstrated good stability and maintained excellent degradation efficiency even across four reaction cycles. Furthermore, the activation mechanism and the intermediates produced during the decomposition course of RhB by MMCCN/PMS/vis system were analyzed and elucidated. A double S-scheme heterojunctions was responsible for efficient separation of photo-induced electron-hole pairs. This work presents a novel method in the construction of double S-scheme heterojunctions for PMS activation which is expected to find wide applications in wastewater treatment and environmental remediation.

摘要

构建半导体异质结是光催化降解污染物过程中电荷分离的有效途径。本研究通过简单的煅烧方法制备了一种新型的MoS@MoO/(Cu/g-CN)三元复合材料(MMCCN)。所制备的复合材料在活化过一硫酸盐(PMS)降解罗丹明B(RhB)方面表现出优异的性能。活性测试结果表明,在可见光照射40分钟的条件下,复合材料光催化剂(0.1 g·L)和PMS(0.1 g·L)的协同作用能有效去除99.41%的RhB(10 mg·L,10 mL)。其反应速率常数分别比Cu/g-CN、MoO和MoS高出3.56倍、17.30倍和11.73倍。根据密度泛函理论(DFT)计算了半导体的晶体结构、带隙和态密度(DOS)。自由基捕获试验和电子自旋共振光谱证实,O₂⁻、¹O₂和h⁺是参与RhB分解的主要活性物种。该三元复合材料表现出良好的稳定性,即使经过四个反应循环仍保持优异的降解效率。此外,还对MMCCN/PMS/vis体系在RhB分解过程中的活化机制和产生的中间体进行了分析和阐释。双S型异质结负责光生电子-空穴对的有效分离。这项工作提出了一种构建用于PMS活化的双S型异质结的新方法,有望在废水处理和环境修复中得到广泛应用。

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