Boosting CO desorption on dual active site electrocatalysts for CO2 reduction to produce tunable syngas

• Published in: Cell reports physical science Vol. 3; no. 1; p. 100703
• Main Authors: Hua, Yani, Zhang, Baowen, Hao, Wenbin, Gao, Zhan
• Format: Journal Article
• Language: English
• Published: Elsevier Inc 19.01.2022
• Subjects: CO2 reduction reaction; dual active sites; electrocatalyst; single-atom catalysts; tunable syngas; single-atom catalysts; tunable syngas; electrocatalyst; CO2 reduction reaction; dual active sites
• ISSN: 2666-3864; 2666-3864
• DOI: 10.1016/j.xcrp.2021.100703

The electrochemical conversion of CO2 to generate syngas (H2 and CO) is regarded as a promising alternative technique to facilitate CO2 reduction in the ambient atmosphere. However, it is still a great challenge to acquire high catalytic activity with an adjustable H2/CO ratio over a wide range. Here, we construct an electrocatalyst with Fe-containing dual active sites on N-doped porous carbon (Fe/FeN4C) to promote a CO2 reduction reaction for tunable syngas production. The Fe/FeN4C catalysts have a positive onset potential (−0.18 VRHE), approximately 100% of the sum of the Faradaic efficiency (FE) of CO and H2, a high total current density (>39.33 mA cm−2), and a wide H2/CO ratio (1.09∼7.08). Density functional-theory calculations suggest that the Fe single atoms dispersed into the N-doped carbon structure, along with the incorporation of Fe nanoparticles, may decrease the adsorption energy of ∗CO, thus synergistically enhancing the catalytic activity. [Display omitted] Fe/FeN4C serves as a dual active site catalyst for CO2RR to syngasThe Fe/FeN4C catalyst displays superior CO2RR performance toward syngasDFT study confirms the decrease in ∗CO adsorption energy benefits syngas production There is interest in developing active catalysts for the electrochemical conversion of carbon dioxide to syngas with a tunable H2/CO ratio. Here, Hua et al. report Fe-containing, N-doped, porous carbon to promote CO2 reduction for tunable syngas production.