Heat-Assisted Visible Light Catalytic PMS for Diclofenac Degradation: Mn-Doped g-C3N4 Catalysts and Synergistic Catalytic Mechanism

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2024-09-13 DOI:10.1007/s10562-024-04817-5

Qinglu Yuan, Peize Wang, Mengjie Fan, Yuan Xu, Yingwen Chen

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Abstract

Different manganese salt precursor-doped g-C₃N₄ catalysts prepared by the mixed calcination method were applied in the heat-assisted visible light catalytic peroxymonosulfate (PMS) activation (Heat/Vis/PMS) system for the degradation of diclofenac (DCF). Under this Heat/Vis/PMS system, the CN-Mn-S catalyst using MnSO₄ as the manganese salt precursor showed the optimal DCF degradation efficiency (96.9%) with the fastest reaction rate (0.1607 min⁻¹). Besides, with the advantages of large specific surface area, high Mn₃O₄ generation, and good visible light absorption performance, CN-Mn-S catalyst also maintained excellent catalytic activity after five cycles. Electron paramagnetic resonance (EPR) analysis revealed that the generation of active species with relatively high contribution to DCF degradation, including generation of superoxide anion (O₂·⁻) and singlet oxygen (¹O₂), were significantly increased in the CN-Mn-S/Heat/Vis/PMS system. Meanwhile, combined with the analysis of influence factor experiments and the DCF degradation characteristics, the CN-Mn-S/Heat/Vis/PMS system was able to maintain excellent DCF degradation ability in complex environments. This work provides a new idea for the application of PMS in real environment.

Graphical Abstract

Abstract Image

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热辅助可见光催化 PMS 降解双氯芬酸：掺锰 g-C3N4 催化剂和协同催化机理

将混合煅烧法制备的不同掺杂锰盐前驱体的 g-C3N4 催化剂应用于热辅助可见光催化过一硫酸盐（PMS）活化（Heat/Vis/PMS）体系，用于降解双氯芬酸（DCF）。在该 Heat/Vis/PMS 系统下，以 MnSO4 为锰盐前驱体的 CN-Mn-S 催化剂表现出最佳的 DCF 降解效率（96.9%）和最快的反应速率（0.1607 min-1）。此外，CN-Mn-S 催化剂还具有比表面积大、Mn3O4 生成量高、可见光吸收性能好等优点，经过五个循环后仍能保持良好的催化活性。电子顺磁共振（EPR）分析表明，CN-Mn-S/Heat/Vis/PMS体系中对DCF降解贡献率较高的活性物种，包括超氧阴离子（O2--）和单线态氧（1O2）的生成显著增加。同时，结合影响因素实验和 DCF 降解特性分析，CN-Mn-S/Heat/Vis/PMS 体系能够在复杂环境中保持优异的 DCF 降解能力。这项工作为 PMS 在实际环境中的应用提供了新思路。

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.