Iron clusters boosted performance in electrocatalytic carbon dioxide conversion
2020
Wu, Dongchuang | Wang, Xinyue | Shi, Linghao | Jiang, Kaiyue | Wang, Mengjia | Lu, Chenbao | Chen, Zhenying | Liu, Pan | Zhang, Jichao | Tranca, Diana | Hou, Yang | Chen, Yu | Zhuang, Xiaodong
Metal clusters with exposed atomic interfaces and unique electronic structures have received considerable attention in heterogeneous catalysis. However, their potential application in the electrocatalytic CO₂ reduction reaction (CO₂RR) remains very challenging because metal clusters tend to drive the competitive hydrogen evolution reaction. In this study, we prepared Fe-cluster sites with positive valence anchored on ordered mesoporous carbon materials for use as an efficient and durable electrocatalyst in carbon dioxide electroreduction. The as-prepared catalyst exhibits high selectivity, with a CO faradaic efficiency of higher than 98% at a low overpotential of 0.37 V, and retains 98.5% of its initial selectivity after 50 h of electrolysis in 0.5 M KHCO₃. In addition, the as-prepared catalyst exhibits enhanced selectivity of more than 95% from −0.5 to −0.8 V in 0.1 M KHCO₃, has 98.6% CO faradaic efficiency at a low overpotential of 0.49 V, and retains 99% of its initial selectivity after 50 h of electrolysis, thus outperforming state-of-the-art Fe–N-based single-atom catalysts. Density functional theory calculations revealed that the atomic interfaces on the Fe clusters reduce the reaction barrier for the *COOH intermediate, thus contributing to the rapid transformation of CO₂ molecules and resulting in excellent catalytic performance.
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