Attenuating metal-substrate conjugation in atomically dispersed nickel catalysts for electroreduction of CO2 to CO

Qiyou Wang, Kang Liu, Kangman Hu, Chao Cai, Huangjingwei Li, Hongmei Li, Matias Herran, Ying-Rui Lu, Ting-Shan Chan, Chao Ma, Junwei Fu, Shiguo Zhang, Ying Liang, Emiliano Cortés () and Min Liu ()
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Qiyou Wang: Central South University
Kang Liu: Central South University
Kangman Hu: Central South University
Chao Cai: Central South University
Huangjingwei Li: Central South University
Hongmei Li: Central South University
Matias Herran: Ludwig-Maximilians-Universität München
Ying-Rui Lu: National Synchrotron Radiation Research Center
Ting-Shan Chan: National Synchrotron Radiation Research Center
Chao Ma: Hunan University
Junwei Fu: Central South University
Shiguo Zhang: Hunan University
Ying Liang: Central South University of Forestry and Technology
Emiliano Cortés: Ludwig-Maximilians-Universität München
Min Liu: Central South University

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Atomically dispersed transition metals on carbon-based aromatic substrates are an emerging class of electrocatalysts for the electroreduction of CO2. However, electron delocalization of the metal site with the carbon support via d-π conjugation strongly hinders CO2 activation at the active metal centers. Herein, we introduce a strategy to attenuate the d-π conjugation at single Ni atomic sites by functionalizing the support with cyano moieties. In situ attenuated total reflection infrared spectroscopy and theoretical calculations demonstrate that this strategy increases the electron density around the metal centers and facilitates CO2 activation. As a result, for the electroreduction of CO2 to CO in aqueous KHCO3 electrolyte, the cyano-modified catalyst exhibits a turnover frequency of ~22,000 per hour at −1.178 V versus the reversible hydrogen electrode (RHE) and maintains a Faradaic efficiency (FE) above 90% even with a CO2 concentration of only 30% in an H-type cell. In a flow cell under pure CO2 at −0.93 V versus RHE the cyano-modified catalyst enables a current density of −300 mA/cm2 with a FE above 90%.

Date: 2022
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DOI: 10.1038/s41467-022-33692-0

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