Nano-Micro Letters

A Universal Principle to Accurately Synthesize Atomically Dispersed Metal-N4 Sites for CO2 Electroreduction

Wanzhen Zheng1, 3, Feng Chen2, Qi Zeng1, Zhongjian Li1, Bin Yang1, 4, Lecheng Lei1, 4, Qinghua Zhang6, Feng He3, Xilin Wu2, *, Yang Hou1, 4, 5, *

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Nano-Micro Lett. (2020) 12: 108

First Online: 09 May 2020 (Communication)

DOI:10.1007/s40820-020-00443-z

*Corresponding author. E-mail: yhou@zju.edu.cn (Yang Hou); dbwxl@zjnu.cn (Xilin Wu)

 

Abstract

 


Toc

Atomically dispersed metal-nitrogen sites anchored carbon materials have been developed as effective catalysts for CO2 electroreduction (CO2ER), but they still suffer from the imprecisely control of type and coordination number of N atoms bonded with central metal. Herein, we develop a family of single metal atom bonded by N atoms anchored on carbons (SAs-M-N-C, M = Fe, Co, Ni, Cu) for CO2ER, which composed of accurate pyrrole-type M-N4 structures with isolated metal atom coordinated by four pyrrolic N atoms. Benefitting from atomically coordinated environment and specific selectivity of M-N4 centers, SAs-Ni-N-C exhibits superior CO2ER performance with onset potential of -0.3 V, CO Faradaic efficiency (F.E.) of 98.5% at -0.7 V, along with low Tafel slope of 115 mV dec-1 and superior stability of 50 h, exceeding all the previously reported M-N-C electrocatalysts for CO2-to-CO conversion. Experimental results manifest that the different intrinsic activities of M-N4 structures in SAs-M-N-C result in the corresponding sequence of Ni > Fe > Cu > Co for CO2ER performance. An integrated Zn-CO2 battery with Zn foil and SAs-Ni-N-C is constructed to simultaneously achieve CO2-to-CO conversion and electric energy output, which delivers a peak power density of 1.4 mW cm-2 and maximum CO F.E. of 93.3%.


 

Keywords

Atomic dispersion, Pyrrole-type metal-N4 structure, Catalytic site, CO2 electroreduction, Zn-CO2 battery

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