Efficient and Robust Carbon Dioxide Electroreduction Enabled by Atomically Dispersed Snδ+ Sites

Advanced Materials
Xiaolong ZuYi Xie

Abstract

Electrocatalytic CO2 reduction at considerably low overpotentials still remains a great challenge. Here, a positively charged single-atom metal electrocatalyst to largely reduce the overpotentials is designed and hence CO2 electroreduction performance is accelerated. Taking the metal Sn as an example, kilogram-scale single-atom Snδ+ on N-doped graphene is first fabricated by a quick freeze-vacuum drying-calcination method. Synchrotron-radiation X-ray absorption fine structure and high-angle annular dark-field scanning transmission electron microscopy demonstrate the atomically dispersed Sn atoms are positively charged, which enables CO2 activation and protonation to proceed spontaneously through stabilizing CO2•- * and HCOO- *, affirmed by in situ Fourier transform infrared spectra and Gibbs free energy calculations. Furthermore, N-doping facilitates the rate-limiting formate desorption step, verified by the decreased desorption energy from 2.16 to 1.01 eV and the elongated SnHCOO- bond length. As an result, single-atom Snδ+ on N-doped graphene exhibits a very low onset overpotential down to 60 mV for formate production and shows a very large turnover frequency up to 11930 h-1 , while its electroreduction activity proceeds wit...Continue Reading

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Citations

Oct 2, 2019·Chemical Society Reviews·Huilong FeiXiangfeng Duan
Jul 10, 2020·Advanced Materials·Minhan LiJianping Yang
Sep 2, 2020·Chemical Society Reviews·Lulu LiJinlong Gong
Jan 13, 2021·Nature Nanotechnology·Richard I MaselCurtis P Berlinguette
Feb 25, 2021·Chemical Society Reviews·Genxiang WangLiming Dai
Dec 15, 2020·Angewandte Chemie·Huabin ZhangXiong Wen David Lou
Jul 10, 2021·Small·Bingxing ZhangWenping Sun
Nov 26, 2020·Accounts of Chemical Research·Xiaodong LiYi Xie
Nov 3, 2020·Chemical Reviews·Yuxuan WangChao Wang
Jun 17, 2020·Journal of the American Chemical Society·Lili HanHuolin L Xin
Jun 17, 2020·ACS Nano·Fizza NaseemZongyou Yin
Sep 29, 2020·Chemical Reviews·Janis Timoshenko, Beatriz Roldan Cuenya
Dec 21, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Dong FangCheng Wang

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