Electrochemical Conversion of CO₂ to Syngas with Controllable CO/H₂ 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.

The electrochemical CO2 reduction reaction (CO2RR) to yield synthesis gas (syngas, CO and H2) has been considered as a promising method to realize the net reduction in CO2 emission. However, it is challenging to balance the CO2RR activity and the CO/H2 ratio. To address this issue, nitrogen‐doped carbon supported single‐atom catalysts are designed as electrocatalysts to produce syngas from CO2RR. While Co and Ni single‐atom catalysts are selective in producing H2 and CO, respectively, electrocatalysts containing both Co and Ni show a high syngas evolution (total current >74 mA cm−2) with CO/H2 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 H2 and CO evolution. The results present a useful case on how non‐precious transition metal species can maintain high CO2RR activity with tunable CO/H2 ratios.

SYNTHESIS gas; WATER gas shift reactions; STEAM reforming; CATALYST supports; ELECTROLYTIC reduction; DENSITY functional theory; OXYGEN reduction; CATALYSTS

Angewandte Chemie, 2020, Vol 132, Issue 8, p3057

0044-8249

Academic Journal

10.1002/ange.201912719