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Adv Mater. 2019 Apr;31(15):e1808135. doi: 10.1002/adma.201808135. Epub 2019 Feb 21.

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

Author information

1
Hefei National Laboratory for Physical Science at Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
2
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, 230029, P. R. China.

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 without deactivation even after 200 h. This work offers a new pathway for manipulating electrocatalytic performance.

KEYWORDS:

CO2 electroreduction; overpotential; robust; single-atom

PMID:
30790366
DOI:
10.1002/adma.201808135

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