Yuan Fufa, Wang Xin, Ma Tao, Fan Jianhua, Lai Xiaoyong, Liu Yingtao
State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, National Demonstration Center for Experimental Chemistry Education, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, China.
State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, National Demonstration Center for Experimental Chemistry Education, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, China.
J Colloid Interface Sci. 2024 Aug;667:291-302. doi: 10.1016/j.jcis.2024.04.078. Epub 2024 Apr 15.
Single atom metal-nitrogen-carbon materials have emerged as remarkably potent catalysts, demonstrating unprecedented potential for the photo-driven reduction of CO. Herein, a unique Cu@g-CN catalyst obtained by cooperation of single atom Cu and nitrogen-rich g-CN is proposed. The particular CuN diatomic active sites (DAS) in Cu@g-CN contribute to the formation of highly stable CuOCN adsorption, a key configuration for CO activation and CC coupling. The synergistic diatomic active sites interaction is found responsible for the efficient photoreduction of CO to CH which has been demonstrated in our Gibbs free energy calculation and COHP analysis. The CO activation mechanism was studied, the charge density difference and DOS analysis show that the low oxidation state Cu atom significantly affects the electronic structure of g-CN and then enhance the catalytic activity of CO hydrogenation.
单原子金属-氮-碳材料已成为极具潜力的催化剂，在光驱动还原CO方面展现出前所未有的潜力。在此，提出了一种通过单原子Cu与富氮g-CN协同作用获得的独特Cu@g-CN催化剂。Cu@g-CN中特殊的CuN双原子活性位点（DAS）有助于形成高度稳定的CuOCN吸附，这是CO活化和C-C偶联的关键构型。在我们的吉布斯自由能计算和COHP分析中已证明，双原子活性位点的协同相互作用负责将CO高效光还原为CH。研究了CO活化机制，电荷密度差和态密度分析表明，低氧化态的Cu原子显著影响g-CN的电子结构，进而增强了CO加氢的催化活性。
