Carbon nitride with grafted molecular as electron acceptor and active site to achieve efficient photo-activated peroxymonosulfate for organic pollutants removal

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-01-04 DOI:10.1016/j.apcatb.2024.123693

Ling Li , Hao Zeng , Rongdi Tang , Zhanpeng Zhou , Sheng Xiong , Wenbo Li , Ying Huang , Yaocheng Deng

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Abstract

The effective activation of peroxymonosulfate (PMS) by polymer carbon nitride (PCN) is hampered by the unpredictable movement and rapid recombination of photocarriers. In this study, niacin served as a beneficial modifier to help constructed the directional electron transfer pathway from the center to the edge in the synthesized PCN catalyst (UCNNA) for efficient PMS activation. The UCNNA/PMS/vis shows the highest kinetic constants (0.050 min⁻¹), which is 2.9-fold increase over the PCN/PMS/vis. The experiments and theoretical calculations indicated that niacin as electron acceptor group prevents the recombination of photocarriers in-plane. Simultaneously, niacin can serve as PMS adsorption site, further facilitating electron transfer and the ¹O₂ generation. Mass spectrometry analysis and Fukui index calculations confirm the priority of lateral chain oxidation (¹O₂ attack site) during atrazine degradation. These results provide new insights into rational design of metal-free catalysts/PMS/vis system, as well as providing guidance and theoretical support for atrazine degradation mechanisms.

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以接枝分子为电子受体和活性位点的氮化碳实现高效光活化过一硫酸盐去除有机污染物的功能

聚合物氮化碳（PCN）对过一硫酸盐（PMS）的有效活化受到光载体不可预测的移动和快速重组的阻碍。在本研究中，烟酸作为一种有益的改性剂，帮助构建了合成 PCN 催化剂（UCNNA）中从中心到边缘的定向电子转移途径，从而实现了 PMS 的高效活化。UCNNA/PMS/vis 的动力学常数最高（0.050 min-1），是 PCN/PMS/vis 的 2.9 倍。实验和理论计算表明，烟酸作为电子受体基团可以阻止光载流子在平面内重组。同时，烟酸可以作为 PMS 的吸附位点，进一步促进电子转移和 1O2 的生成。质谱分析和福井指数计算证实了阿特拉津降解过程中横向链氧化（1O2 攻击位点）的优先性。这些结果为无金属催化剂/PMS/vis 系统的合理设计提供了新的见解，同时也为阿特拉津的降解机理提供了指导和理论支持。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.