Guo Yanling, Zhang Lisu, Zou Yanbo, Wang Xingguo, Ning Qian
School of Physics and Electronic Engineering, Xinjiang Normal University, Urumqi 830054, China.
Xinjiang Key Laboratory for Luminescence Minerals and Optical Functional Materials, Urumqi 830054, China.
Nanomaterials (Basel). 2025 Mar 15;15(6):445. doi: 10.3390/nano15060445.
In recent years, driven by the swift progress in nanotechnology and catalytic science, researchers in the field of physical chemistry have been vigorously exploring novel catalysts designed to enhance the efficiency and selectivity of a broad spectrum of chemical reactions. Against this backdrop, Cu clusters supported on defective graphene (Cu@GR, where = 5, 6) function as two-dimensional nanocatalysts, demonstrating exceptional catalytic activity in the electrochemical reduction of carbon dioxide (CORR). A comprehensive investigation into the catalytic properties of these materials has been undertaken using density functional theory (DFT) calculations. By tailoring the configuration of Cu@GR, specific reduction products such as CH and CHOH can be selectively produced. The product selectivity is quantitatively analyzed through free energy calculations. Remarkably, the Cu@GR catalyst enables the electrochemical reduction of CO to CH with a significantly low overpotential of -0.31 eV. Furthermore, the overpotential of the hydrogen evolution reaction (HER) is higher than that of the conversion of CO to CH; hence, the HER is unlikely to interfere and impede the efficiency of CH production. This study demonstrates that Cu@GR offers low overpotential and high catalytic efficiency, providing a theoretical foundation for the design and experimental synthesis of composite nanocatalysts.
近年来，在纳米技术和催化科学迅速发展的推动下，物理化学领域的研究人员一直在积极探索旨在提高广泛化学反应效率和选择性的新型催化剂。在此背景下，负载在缺陷石墨烯上的铜簇（Cu@GR，其中 = 5, 6）作为二维纳米催化剂，在二氧化碳电化学还原（CORR）中表现出卓越的催化活性。已使用密度泛函理论（DFT）计算对这些材料的催化性能进行了全面研究。通过调整Cu@GR的构型，可以选择性地产生特定的还原产物，如CH和CHOH。通过自由能计算对产物选择性进行了定量分析。值得注意的是，Cu@GR催化剂能够以低至 -0.31 eV的过电位将CO电化学还原为CH。此外，析氢反应（HER）的过电位高于CO转化为CH的过电位；因此，HER不太可能干扰和阻碍CH的生产效率。这项研究表明，Cu@GR具有低过电位和高催化效率，为复合纳米催化剂的设计和实验合成提供了理论基础。
