Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single‐Atom Catalysts

He, Qun; Liu, Daobin; Lee, Ji Hoon; Liu, Yumeng; Xie, Zhenhua; Hwang, Sooyeon; Kattel, Shyam; Song, Li; Chen, Jingguang G.

doi:10.1002/anie.201912719

Electrochemical Conversion of CO ₂ to Syngas with Controllable CO/H ₂ Ratios over Co and Ni Single‐Atom Catalysts

Journal Article · Thu Jan 09 00:00:00 EST 2020 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201912719· OSTI ID:1581851

^[1]; Liu, Daobin ^[2]; ^[3]; Liu, Yumeng ^[3]; ^[4]; ^[5]; Kattel, Shyam ^[6]; Song, Li ^[7]; ^[4]

National Synchrotron Radiation Laboratory CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230029 China, Department of Chemical Engineering Columbia University New York NY 10027 USA
School of Materials Science and Engineering Nanyang Technological University Singapore 639798 Singapore
Department of Chemical Engineering Columbia University New York NY 10027 USA
Department of Chemical Engineering Columbia University New York NY 10027 USA, Chemistry Division Brookhaven National Laboratory Upton NY 11973 USA
Center for Functional Nanomaterials Brookhaven National Laboratory Upton NY 11973 USA
Department of Physics Florida A&,M University Tallahassee FL 32307 USA
National Synchrotron Radiation Laboratory CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei Anhui 230029 China

Abstract

The electrochemical CO ₂ reduction reaction (CO ₂ RR) to yield synthesis gas (syngas, CO and H ₂ ) has been considered as a promising method to realize the net reduction in CO ₂ emission. However, it is challenging to balance the CO ₂ RR activity and the CO/H ₂ ratio. To address this issue, nitrogen‐doped carbon supported single‐atom catalysts are designed as electrocatalysts to produce syngas from CO ₂ RR. While Co and Ni single‐atom catalysts are selective in producing H ₂ and CO, respectively, electrocatalysts containing both Co and Ni show a high syngas evolution (total current >74 mA cm ⁻² ) with CO/H ₂ ratios (0.23–2.26) that are suitable for typical downstream thermochemical reactions. Density functional theory calculations provide insights into the key intermediates on Co and Ni single‐atom configurations for the H ₂ and CO evolution. The results present a useful case on how non‐precious transition metal species can maintain high CO ₂ RR activity with tunable CO/H ₂ ratios.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0009476

OSTI ID:: 1581851

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 8 Vol. 59; ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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