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构建具有双位点的纳米异质结构以促进羟基自由基激活并调控自由基转化

Constructing Nano-Heterostructure with Dual-Site to Boost HO Activation and Regulate the Transformation of Free Radicals.

作者信息

Shang Denghui, Wang Siyu, Li Jialu, Zhan Sihui, Hu Wenping, Li Yi

机构信息

Key Laboratory of Organic Integrated Circuits, Ministry of Education & Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.

College of Environmental Science and Engineering, Nankai University, Tianjin, 300071, China.

出版信息

Small. 2024 Aug;20(31):e2311984. doi: 10.1002/smll.202311984. Epub 2024 Mar 10.

DOI:10.1002/smll.202311984
PMID:38461526
Abstract

A major issue with Fenton-like reaction is the excessive consumption of HO caused by the sluggish regeneration rate of low-valent metal, and how to improve the activation efficiency of HO has become a key in current research. Herein, a nano-heterostructure catalyst (1.0-MnCu/C) based on nano-interface engineering is constructed by supporting Cu and MnO on carbon skeleton, and its kinetic rate for the degradation of tetracycline hydrochloride is 0.0436 min, which is 2.9 times higher than that of Cu/C system (0.0151 min). The enhancement of removal rate results from the introduced Mn species can aggregate and transfer electrons to Cu sites through the electron bridge Mn-N/O-Cu, thus preventing Cu from oxidizing HO to form O , and facilitating the reduction of Cu and generating more reactive oxygen species (O and ·OH) with stronger oxidation ability, resulting in HO utilization efficiency is 1.9 times as much as that of Cu/C. Additionally, the good and stable practical application capacity in different bodies demonstrates that it has great potential for practical environmental remediation.

摘要

类芬顿反应的一个主要问题是低价金属再生速率缓慢导致羟基自由基(HO)过度消耗,如何提高HO的活化效率已成为当前研究的关键。在此,通过在碳骨架上负载铜和MnO构建了一种基于纳米界面工程的纳米异质结构催化剂(1.0-MnCu/C),其降解盐酸四环素的动力学速率为0.0436 min⁻¹,比Cu/C体系(0.0151 min⁻¹)高2.9倍。去除率的提高源于引入的锰物种可以通过电子桥Mn-N/O-Cu聚集并将电子转移到铜位点,从而防止铜将HO氧化形成氧气,促进铜的还原并产生更多具有更强氧化能力的活性氧物种(O₂和·OH),使得HO的利用效率是Cu/C的1.9倍。此外,在不同体系中良好且稳定的实际应用能力表明其在实际环境修复中具有巨大潜力。

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