Engineering Unsaturated Cu 1 –O 3 Coordination to Boost Oxygen Species Activation for Low-Temperature Catalysis in CO Oxidation

作者：Yadi Wang, Zeyu Jiang, Fan Dang, Chaoqian Ai, Jialei Wan, Chunli Ai, Yani Wu, Chi Ma, Mingjiao Tian, Xu Ha, Reem Albilali, Weisheng Guan, Hongna Zhang, Chi He · 发表于：JACS Au · 年份：2025 · DOI：10.1021/jacsau.4c01149 · 被引用次数：6 · 研究领域：Catalytic Processes in Materials Science、Catalysis and Oxidation Reactions、Copper-based nanomaterials and applications

High Resolution Image Download MS PowerPoint Slide The activation of lattice oxygen at low temperatures is essential for heterogeneous catalytic oxidation, but exactly how this is achieved by adjusting the coordination structure of atomic sites is still elusive. Herein, the Cu 1 O 3 –CeO 2 catalyst with highly dispersed unsaturated Cu 1 –O 3 coordination was creatively engineered, which remarkably enhanced the low-temperature oxidation of CO (a typical model reaction) from 12% to 90% at 66 °C compared to conventional CuCeO x catalyst. The preservation of atomic coordination-deficient Cu sites enables the transfer of electron cloud density from Cu atoms to O atoms, hence, facilitating the activation of lattice oxygen. Further electron transfer from O atom to Cu species results in charge back-donation to form sufficient Cu + and metal per-oxy species, contributing to weaken O–O bonds. We determined that the increasing number of electron donors induced by unsaturated atomic Cu 1 –O 3 coordination is an efficient strategy to develop highly active and stable catalysts for lattice oxygen activation. The catalyst synthesis strategies and oxygen activation mechanism demonstrated in this work provide a generalizable platform for the future design of well-defined functional catalysts for low-temperature oxidation reactions.