CuO-CeO催化剂氧化还原反应中表面碳物种的亲电性

Kang Liqun, Wang Bolun, Güntner Andreas T, Xu Siyuan, Wan Xuhao, Liu Yiyun, Marlow Sushila, Ren Yifei, Gianolio Diego, Tang Chiu C, Murzin Vadim, Asakura Hiroyuki, He Qian, Guan Shaoliang, Velasco-Vélez Juan J, Pratsinis Sotiris E, Guo Yuzheng, Wang Feng Ryan

Department of Chemical Engineering, University College London, London, WC1E 7JE, UK.

Particle Technology Laboratory, Institute of Process Engineering, Department of Mechanical and Process Engineering, ETH Zürich, 8092, Zürich, Switzerland.

Angew Chem Int Ed Engl. 2021 Jun 21;60(26):14420-14428. doi: 10.1002/anie.202102570. Epub 2021 Apr 8.

Electronic metal-support interactions (EMSI) describe the electron flow between metal sites and a metal oxide support. It is generally used to follow the mechanism of redox reactions. In this study of CuO-CeO redox, an additional flow of electrons from metallic Cu to surface carbon species is observed via a combination of operando X-ray absorption spectroscopy, synchrotron X-ray powder diffraction, near ambient pressure near edge X-ray absorption fine structure spectroscopy, and diffuse reflectance infrared Fourier transform spectroscopy. An electronic metal-support-carbon interaction (EMSCI) is proposed to explain the reaction pathway of CO oxidation. The EMSCI provides a complete picture of the mass and electron flow, which will help predict and improve the catalytic performance in the selective activation of CO , carbonate, or carbonyl species in C1 chemistry.

电子-金属-载体相互作用（EMSI）描述了金属位点与金属氧化物载体之间的电子流动。它通常用于追踪氧化还原反应的机理。在这项关于CuO-CeO氧化还原的研究中，通过原位X射线吸收光谱、同步辐射X射线粉末衍射、近常压近边X射线吸收精细结构光谱和漫反射红外傅里叶变换光谱的组合，观察到了从金属Cu到表面碳物种的额外电子流。提出了一种电子-金属-载体-碳相互作用（EMSCI）来解释CO氧化的反应途径。EMSCI提供了质量和电子流动的完整图景，这将有助于预测和改善C1化学中CO、碳酸盐或羰基物种选择性活化的催化性能。