哈尔滨工业大学马军团队提出了MXene基金属阵列的不对称配位工程及其在快速水净化中的应用。这一研究成果发表在2025年12月1日出版的国际学术期刊《德国应用化学》上。

高价金属氧化物（HVMOS）在水净化中具有重要的应用价值，因为它们打破了传统的基于自由基的高级氧化工艺的活性-选择性权衡。

然而，由于难以精确设计合适的高负载活性位点，通过多相反应制备定向HVMOS一直是一个挑战。

本文提出了一种简单的不对称含氧配位策略来激活V₂C MXene中的惰性金属阵列，该策略可以有效地激活过氧单硫酸盐（PMS）来选择性地生成HVMOS。邻近V点之间独特的超短距离（2.36Å）不对称配位的MXene产生了独特的拓扑交感电场（TSEF），实现了高效的PMS活化和超快的水污染物氧化（k_obs = 1498.33 min^-1M^-1）。机理研究揭示了一条从PMS到V₂C通过短程双金属氧桥的单电子转移新途径，显著降低了TSEF促进HVMOS生成的能量势垒。非自由基体系在不同的实际水基质和长期运行中表现出较强的抗干扰能力和良好的稳定性。

附：英文原文

Title: Asymmetric Coordination Engineering of MXene-Based Metal Arrays for Oriented Generation of High-Valent Metal-Oxo Species from Peroxymonosulfate for Fast Water Decontamination

Author: Zhifeng Li, Xiaoyue Ji, Qingbao Li, Yufei Zhen, Shishu Zhu, Xing Xu, Wei Wang, Xiaoguang Duan, Zhiqiang Sun, Jun Ma

Issue&Volume: 2025-12-01

Abstract: High-valent metal-oxo species (HVMOS) are appealing for water purification because they break the activity-selectivity trade-off of conventional radical-based advanced oxidation processes. However, oriented HVMOS generation via heterogeneous reactions has been challenging because of the difficulty in the precise design of favourable and high-loading active sites. Herein, a facile asymmetric oxygen-containing coordination strategy was developed to activate inert metal arrays in V2C MXene, which could effectively activate peroxymonosulfate (PMS) to selectively generate HVMOS. The unique ultrashort-range distance between neighboring V sites (2.36Å) in MXene with asymmetric coordination generated a distinctive topological sympathetic electric field (TSEF), which enabled efficient PMS activation and ultrafast oxidation of water pollutants (kobs = 1498.33 min1M1). Mechanistic studies revealed a new single-electron-transfer pathway from PMS to V2C through short-range bimetallic oxygen bridges, significantly reducing the energy barrier of HVMOS generation promoted by TSEF. The nonradical system exhibited robust anti-interference capacity and excellent stability in different real water matrices and long-term operations.

DOI: 10.1002/anie.202522714

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202522714