Dynamic Activation of Adsorbed Intermediates via Axial Traction for the Promoted Electrochemical CO2 Reduction.
Regulating the local environment and structure of metal center coordinated by nitrogen ligands (M-N4 ) to accelerate overall reaction dynamics of the electrochemical CO2 reduction reaction (CO2 RR) has attracted extensive attention. Herein, we develop an axial traction strategy to optimize the electronic structure of the M-N4 moiety and construct atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom, which are embedded within the carbon matrix (Ni-N4 -O/C). The Ni-N4 -O/C electrocatalyst exhibited excellent CO2 RR performance with a maximum CO Faradic efficiency (FE) close to 100 % at -0.9 V. The CO FE could be maintained above 90 % in a wide range of potential window from -0.5 to -1.1 V. The superior CO2 RR activity is due to the Ni-N4 -O active moiety composed of a Ni-N4 site with an additional oxygen atom that induces an axial traction effect.
['Wang|Xinyue|X|', 'Wang|Yu|Y|', 'Sang|Xiahan|X|', 'Zheng|Wanzhen|W|', 'Zhang|Shihan|S|', 'Shuai|Ling|L|', 'Yang|Bin|B|', 'Li|Zhongjian|Z|', 'Chen|Jianmeng|J|', 'Lei|Lecheng|L|', 'Adli|Nadia Mohd|NM|', 'Leung|Michael K H|MKH|', 'Qiu|Ming|M|', 'Wu|Gang|G|', 'Hou|Yang|Y|http://orcid.org/0000-0001-9795-8503']
axial traction dynamic understanding electrochemical CO2RR single-atom catalysts