Artificial manganese nanozyme for nonradical activation of periodate toward pH-universal water decontamination

IF 11.6 Q1 CHEMISTRY, PHYSICAL

Chem Catalysis Pub Date : 2025-03-04 DOI:10.1016/j.checat.2025.101299

Minjia Yan, Jiahao Sun, Yujing Chen, Xixian Liu, Bowen Xu, Jianrong Chen, Feng Chen, Qianwei Liang, Shaobin Wang, Xi-Lin Wu, Xiaoguang Duan

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引用次数: 0

Abstract

Single-atom nanozymes (SAzymes), designed to mimic the active centers of natural enzymes, are emerging as a versatile catalytic platform for heterogeneous catalysis. Herein, enzyme-mimicking single-atom manganese (EMSA-Mn) sites supported on graphitic carbon nitride (g-C₃N₄) were constructed, marking a pioneering application of EMSA-Mn-C₃N₄ for periodate (PI; IO₄⁻)-based advanced oxidation processes (AOPs). The EMSA-Mn-C₃N₄/PI system demonstrated remarkable efficiency in eliminating organic micropollutants across a broad pH range (pH 3–11). The positively charged EMSA-Mn sites facilitated the adsorption of the negatively charged IO₄⁻, forming the EMSA-Mn-PI∗ complex, subsequently triggering a direct electron-transfer process (ETP) for oxidation of the organic pollutants. Experimental and theoretical results revealed that the EMSA-Mn site possesses higher intrinsic activity than conventional SA-Mn sites anchored on g-C₃N₄, thereby achieving higher efficiency for PI activation via the ETP. This work provides an advanced design strategy to construct Mn SAzymes for environmental catalysis and deeper insights into the nonradical PI-AOP systems.

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人工锰纳米酶非自由基活化高碘酸盐在ph -通用水净化中的应用

单原子纳米酶（SAzymes）被设计成模拟天然酶的活性中心，正在成为多相催化的多功能催化平台。本文构建了基于石墨氮化碳（g-C3N4）的模拟酶单原子锰（EMSA-Mn）位点，标志着EMSA-Mn- c3n4在高酸盐(PI；基于IO4−的高级氧化工艺（AOPs）。EMSA-Mn-C3N4/PI系统在广泛的pH范围（pH 3-11）内具有显著的去除有机微污染物的效率。带正电的EMSA-Mn位点促进了带负电的IO4−的吸附，形成EMSA-Mn- pi *复合物，随后触发了有机污染物氧化的直接电子转移过程（ETP）。实验和理论结果表明，EMSA-Mn位点比锚定在g-C3N4上的传统SA-Mn位点具有更高的固有活性，从而通过ETP实现更高的PI激活效率。这项工作提供了一种先进的设计策略来构建Mn SAzymes用于环境催化和更深入地了解非自由基PI-AOP系统。

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来源期刊

Chem Catalysis

CiteScore

10.50

自引率

6.40%

发文量

期刊介绍： Chem Catalysis is a monthly journal that publishes innovative research on fundamental and applied catalysis, providing a platform for researchers across chemistry, chemical engineering, and related fields. It serves as a premier resource for scientists and engineers in academia and industry, covering heterogeneous, homogeneous, and biocatalysis. Emphasizing transformative methods and technologies, the journal aims to advance understanding, introduce novel catalysts, and connect fundamental insights to real-world applications for societal benefit.