2025年1月14日出版的《美国化学会杂志》发表了中国科学院大连化物所张波研究小组的最新成果，他们的最新研究提出了悬挂在镍氧化物上单铼原子对葡萄糖的高效电化学氧化。

据介绍，定义良好的单原子催化剂（SACs）是直接比较实验结果和理论计算的理想模型系统，为多相催化过程提供了深刻的见解。然而，由于活性位点的结构演变不可预测，嵌入活性位点可能会在化学反应中产生位阻，因此精确设计和可控合成SACs仍然具有挑战性。

在该文章中，课题组人员提出了NiO支持的具有明确定义的，菲咯啉配位的Re单原子催化剂（SACs）的非热解合成（Re₁-phen/NiO）。多个实验表征和理论计算揭示了孤立的Re原子被悬挂在NiO表面上的想法，由垂直于表面的菲罗啉配体连接。

这种独特的结构为Re₁-phen/NiO SAC提供了强大的激活葡萄糖分子的能力，使得在开放式的反应环境中，完全暴露的Re=O双键可以同时与葡萄糖分子两端的羟基和醛基反应，快速形成葡萄糖酸。

附：英文原文

Title: "Suspended" Single Rhenium Atoms on Nickel Oxide for Efficient Electrochemical Oxidation of Glucose

Author: Xunzhu Jiang, Xianhong Wu, Mingyue Lv, Xiaoli Pan, Hua Wang, Chenyang Li, Meixin Chen, Wei Chen, Bo Zhang, Guangtao Yu, Zhong-Shuai Wu, Botao Qiao, Bin Liu, Fritz E. Kühn, Tao Zhang

Issue&Volume: January 14, 2025

Abstract: Well-defined single-atom catalysts (SACs) serve as ideal model systems for directly comparing experimental results with theoretical calculations, offering profound insights into heterogeneous catalytic processes. However, precisely designing and controllably synthesizing SACs remain challenging due to the unpredictable structure evolution of active sites and generation of embedded active sites, which may bring about steric hindrance during chemical reactions. Herein, we present the precious nonpyrolysis synthesis of Re SACs with a well-defined phenanthroline coordination supported by NiO (Re1-phen/NiO). Multiple experimental characterizations together with theoretical calculations unravel the idea that the isolated Re atoms are suspended on the NiO surface, connected by phenanthroline ligands standing perpendicular to the surface. This unique structure provides the Re1-phen/NiO SAC with a strong capability to activate glucose molecules, enabling fully exposed Re=O double bonds in an open-ended reaction environment to simultaneously react with hydroxyl and aldehyde groups at both ends of the glucose molecule, rapidly forming glucaric acid.

DOI: 10.1021/jacs.4c13368

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c13368