Boosting the Ni-Zn interplay via O/N dual coordination for high-efficiency CO_(2) electroreduction

作     者：Ying Zhang Hailei Jiang Anuj Kumar Hongchuan Zhang Zongge Li Tongxin Xu Yuan Pan Yaqun Wang Zhiming Liu Guoxin Zhang Zifeng Yan Ying Zhang;Hailei Jiang;Anuj Kumar;Hongchuan Zhang;Zongge Li;Tongxin Xu;Yuan Pan;Yaqun Wang;Zhiming Liu;Guoxin Zhang;Zifeng Yan

作者机构：State Key Laboratory of Heavy Oil ProcessingCollege of Chemistry and Chemical EngineeringChina University of Petroleum(East China)QingdaoShandongChina Department of ChemistryInstitute of Humanities and Applied ScienceGLA UniversityMathuraIndia College of Chemistry and Chemical EngineeringLiaocheng UniversityLiaochengShandongChina Al‐Ion Battery Research CenterCollege of Energy Storage TechnologyShandong University of Science and TechnologyQingdaoShandongChina Shandong Engineering Laboratory for Preparation and Application of High‐performance Carbon‐MaterialsCollege of Electromechanical EngineeringQingdao University of Science and TechnologyQingdaoShandongChina 

出 版 物：《Carbon Energy》 (碳能源（英文）)

年 卷 期：2023年第5卷第4期

页      面：68-80页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基　　金：National Natural Science Foundation of China,Grant/Award Number:22071137 Key Projects of China National Key R&D Plan,Grant/Award Number:2018YFE0118200 Key Projects of Shandong Key R&D plan,Grant/Award Number:2019JZZY010506 Taishan Scholar Foundation,Grant/Award Number:tspd20210308 

主　　题：atomic dispersion carbon materials CO_(2)reduction formamide metal-nitrogen-carbon 

摘      要：Design of supportive atomic sites with a controllably adjusted coordinating environment is essential to advancing the reduction of CO_(2) to value-added fuels and chemicals and to achieving carbon ***,atomic Ni(Zn)sites that are uniquely coordinated with ternary Zn(Ni)/N/O ligands were successfully decorated on formamide-derived porous carbon nanomaterials,possibly forming an atomic structure of Ni(N_(2)O_(1))-Zn(N_(2)O_(1)),as studied by combining X-ray photoelectron spectroscopy and X-ray absorption *** the mediation of additional O coordination,the Ni-Zn dual site induces significantly decreased desorption of molecular *** NiZn-NC decorated with rich Ni(N_(2)O_(1))-Zn(N_(2)O_(1))sites remarkably gained97%CO Faraday efficiency over a wide potential range of -0.8 to -1.1 V(relative to reversible hydrogen electrode).Density functional theory computations suggest that the N/O dual coordination effectively modulates the electronic structure of the Ni-Zn duplex and optimizes the adsorption and conversion properties of CO_(2) and subsequent *** from the conventional pathway of using Ni as the active site in the Ni-Zn duplex,it is found that the Ni-neighboring Zn sites in the Ni(N_(2)O_(1))-Zn(N_(2)O_(1))coordination showed much lower energy barriers of the CO_(2) protonation step and the subsequent dehydroxylation step.