Gas Diffusion Strategy for Inserting Atomic Iron Sites into Graphitized Carbon Supports for Unusually High-Efficient CO2 Electroreduction and High-Performance Zn-CO2 Batteries

Tingting Wang; Xiahan Sang; Wanzhen Zheng; Bin Yang; Siyu Yao; Chaojun Lei; Zhongjian Li; Qinggang He; Jianguo Lu; Lecheng Lei; Liming Dai; Yang Hou

doi:10.1002/adma.202002430

Gas Diffusion Strategy for Inserting Atomic Iron Sites into Graphitized Carbon Supports for Unusually High-Efficient CO₂ Electroreduction and High-Performance Zn-CO₂ Batteries

Adv Mater. 2020 Jul;32(29):e2002430. doi: 10.1002/adma.202002430. Epub 2020 Jun 15.

Authors

Tingting Wang¹, Xiahan Sang², Wanzhen Zheng¹, Bin Yang¹, Siyu Yao¹, Chaojun Lei¹, Zhongjian Li¹, Qinggang He¹, Jianguo Lu³, Lecheng Lei^{1

4}, Liming Dai⁵, Yang Hou^{1

4

6}

Affiliations

¹ Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, China.
² Research and Testing Centre of Material, School of Materials Science and Engineering, Wuhan University of Technology, Wuhan, 430070, China.
³ State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China.
⁴ Institute of Zhejiang University - Quzhou, Quzhou, 324000, China.
⁵ School of Chemical Engineering, University of New South Wales, Sydney, NSW, 2052, Australia.
⁶ Ningbo Research Institute, Zhejiang University, Ningbo, 315100, China.

PMID: 32538500
DOI: 10.1002/adma.202002430

Abstract

Emerging single-atom catalysts (SACs) hold great promise for CO₂ electroreduction (CO₂ ER)_, but the design of highly active and cost-efficient SACs is still challenging. Herein, a gas diffusion strategy, along with one-step thermal activation, for fabricating N-doped porous carbon polyhedrons with trace isolated Fe atoms (Fe₁ NC) is developed. The optimized Fe₁ NC/S₁ -1000 with atomic Fe-N₃ sites supported by N-doped graphitic carbons exhibits superior CO₂ ER performance with the CO Faradaic efficiency up to 96% at -0.5 V, turnover frequency of 2225 h^-1 , and outstanding stability, outperforming almost all previously reported SACs based on N-doped carbon supported nonprecious metals. The observed excellent CO₂ ER performance is attributed to the greatly enhanced accessibility and intrinsic activity of active centers due to the increased electrochemical surface area through size modulation and the redistribution of doped N species by thermal activation. Experimental observations and theoretical calculations reveal that the Fe-N₃ sites possess balanced adsorption energies of *COOH and *CO intermediates, facilitating CO formation. A universal gas diffusion strategy is used to exclusively yield a series of dimension-controlled carbon-supported SACs with single Fe atoms while a rechargeable Zn-CO₂ battery with Fe₁ NC/S₁ -1000 as cathode is developed to deliver a maximal power density of 0.6 mW cm^-2 .

Keywords: CO2 electroreduction; Zn-CO2 batteries; atomic Fe-N3 sites; dimension-controlled nanocarbons; gas diffusion strategy.

Abstract

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