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Breaking scaling relations for efficient CO2 electrochemical reduction through dual-atom catalysts
Chemical Science ( IF 7.6 ) Pub Date : 2020/01/06 , DOI: 10.1039/c9sc05236d Yixin Ouyang 1 , Li Shi 1 , Xiaowan Bai 1 , Qiang Li 1 , Jinlan Wang 1
Chemical Science ( IF 7.6 ) Pub Date : 2020/01/06 , DOI: 10.1039/c9sc05236d Yixin Ouyang 1 , Li Shi 1 , Xiaowan Bai 1 , Qiang Li 1 , Jinlan Wang 1
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The electrochemical reduction of CO2 offers an elegant solution to the current energy crisis and carbon emission issues, but the catalytic efficiency for CO2 reduction is seriously restricted by the inherent scaling relations between the adsorption energies of intermediates. Herein, by combining the concept of single-atom catalysts and multiple active sites, we design heteronuclear dual-atom catalysts to break through the stubborn restriction of scaling relations on catalytic activity. Twenty-one kinds of heteronuclear transition-metal dimers are embedded in monolayer C2N as potential dual-atom catalysts. First-principles calculations reveal that by adjusting the components of dimers, the two metal atoms play the role of carbon adsorption sites and oxygen adsorption sites respectively, which results in the decoupling of adsorption energies of key intermediates. Free energy profiles demonstrate that CO2 can be efficiently reduced to CH4 on CuCr/C2N and CuMn/C2N with low limiting potentials of −0.37 V and −0.32 V, respectively. This study suggests that the introduction of multiple active sites into porous two-dimensional materials would provide a great possibility for breaking scaling relations to achieve efficient multi-intermediate electrocatalytic reactions.
中文翻译：
通过双原子催化剂打破比例关系，实现高效 CO2 电化学还原
CO 2的电化学还原为当前的能源危机和碳排放问题提供了一种优雅的解决方案，但CO 2还原的催化效率受到中间体吸附能之间固有的比例关系的严重限制。在此，我们结合单原子催化剂和多个活性位点的概念，设计了异核双原子催化剂，突破了尺度关系对催化活性的顽固限制。二十一种异核过渡金属二聚体嵌入单层C 2 N中作为潜在的双原子催化剂。第一性原理计算表明，通过调整二聚体的组成，两个金属原子分别发挥碳吸附位点和氧吸附位点的作用，从而实现关键中间体吸附能的解耦。自由能曲线表明CO 2可以在CuCr/C 2 N和CuMn/C 2 N上有效地还原为CH 4 ，极限电势分别为-0.37 V和-0.32 V。这项研究表明，在多孔二维材料中引入多个活性位点将为打破尺度关系以实现高效的多中间体电催化反应提供很大的可能性。
更新日期：2020-02-19
中文翻译：
通过双原子催化剂打破比例关系，实现高效 CO2 电化学还原
CO 2的电化学还原为当前的能源危机和碳排放问题提供了一种优雅的解决方案，但CO 2还原的催化效率受到中间体吸附能之间固有的比例关系的严重限制。在此，我们结合单原子催化剂和多个活性位点的概念，设计了异核双原子催化剂，突破了尺度关系对催化活性的顽固限制。二十一种异核过渡金属二聚体嵌入单层C 2 N中作为潜在的双原子催化剂。第一性原理计算表明，通过调整二聚体的组成，两个金属原子分别发挥碳吸附位点和氧吸附位点的作用，从而实现关键中间体吸附能的解耦。自由能曲线表明CO 2可以在CuCr/C 2 N和CuMn/C 2 N上有效地还原为CH 4 ，极限电势分别为-0.37 V和-0.32 V。这项研究表明，在多孔二维材料中引入多个活性位点将为打破尺度关系以实现高效的多中间体电催化反应提供很大的可能性。
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