Boosting CO desorption on dual active site electrocatalysts for CO2 reduction to produce tunable syngas
Yani Hua, Baowen Zhang, Wenbin Hao, Zhan Gao
Abstract
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.