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 

机构地区：[1]State Key Laboratory of Heavy Oil Processing,College of Chemistry and Chemical Engineering,China University of Petroleum(East China),Qingdao,Shandong,China [2]Department of Chemistry,Institute of Humanities and Applied Science,GLA University,Mathura,India [3]College of Chemistry and Chemical Engineering,Liaocheng University,Liaocheng,Shandong,China [4]Al‐Ion Battery Research Center,College of Energy Storage Technology,Shandong University of Science and Technology,Qingdao,Shandong,China [5]Shandong Engineering Laboratory for Preparation and Application of High‐performance Carbon‐Materials,College of Electromechanical Engineering,Qingdao University of Science and Technology,Qingdao,Shandong,China

出　　处：《Carbon Energy》2023年第4期68-80,共13页碳能源（英文）

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。

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 neutralization.Herein,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 spectroscopy.With the mediation of additional O coordination,the Ni-Zn dual site induces significantly decreased desorption of molecular CO.The NiZn-NC decorated with rich Ni(N_(2)O_(1))-Zn(N_(2)O_(1))sites remarkably gained>97%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 intermediates.Different 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.

关 键 词：atomic dispersion carbon materials CO_(2)reduction FORMAMIDE metal-nitrogen-carbon 

分 类 号：O64[理学—物理化学]