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Gas Diffusion Strategy for Inserting Atomic Iron Sites into Graphitized Carbon Supports for Unusually High‐Efficient CO 2 Electroreduction and High‐Performance Zn–CO 2 Batteries
Author(s) -
Wang Tingting,
Sang Xiahan,
Zheng Wanzhen,
Yang Bin,
Yao Siyu,
Lei Chaojun,
Li Zhongjian,
He Qinggang,
Lu Jianguo,
Lei Lecheng,
Dai Liming,
Hou Yang
Publication year - 2020
Publication title -
advanced materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.707
H-Index - 527
eISSN - 1521-4095
pISSN - 0935-9648
DOI - 10.1002/adma.202002430
Subject(s) - materials science , faraday efficiency , adsorption , electrochemistry , carbon fibers , catalysis , chemical engineering , diffusion , doping , nanotechnology , electrode , chemistry , thermodynamics , organic chemistry , optoelectronics , composite material , physics , composite number , engineering
Emerging single‐atom catalysts (SACs) hold great promise for CO 2 electroreduction (CO 2 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 (Fe 1 NC) is developed. The optimized Fe 1 NC/S 1 ‐1000 with atomic Fe‐N 3 sites supported by N‐doped graphitic carbons exhibits superior CO 2 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 CO 2 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‐N 3 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–CO 2 battery with Fe 1 NC/S 1 ‐1000 as cathode is developed to deliver a maximal power density of 0.6 mW cm −2 .