1. Engineering iron carbide catalyst with aerophilic and electron-rich surface for improved electrochemical CO2 reduction.
- Author
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Yan, Jing, Ma, Haiyan, Ni, Jiaqi, Ma, Jinjin, Xu, Junjie, Qi, Jiaou, Zhu, Shufang, and Lu, Lilin
- Subjects
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CEMENTITE , *IRON catalysts , *ELECTROLYTIC reduction , *CARBON dioxide reduction , *CARBON dioxide , *DENSITY functional theory - Abstract
[Display omitted] Highly efficient electrocatalyst for carbon dioxide reduction (CO 2 RR) is desirable for converting CO 2 into carbon-based chemicals and reducing anthropogenic carbon emission. Regulating catalyst surface to improve the affinity for CO 2 and the capability of CO 2 activation is the key to high-efficiency CO 2 RR. In this work, we develop an iron carbide catalyst encapsulated in nitrogenated carbon (SeN-Fe 3 C) with an aerophilic and electron-rich surface by inducing preferential formation of pyridinic-N species and engineering more negatively charged Fe sites. The SeN-Fe 3 C exhibits an excellent CO selectivity with a CO Faradaic efficiency (FE) of 92 % at −0.5 V (vs. RHE) and remarkably enhanced CO partial current density as compared to the N-Fe 3 C catalyst. Our results demonstrate that Se doping reduces the Fe 3 C particle size and improves the dispersion of Fe 3 C on nitrogenated carbon. More importantly, the preferential formation of pyridinic-N species induced by Se doping endows the SeN-Fe 3 C with an aerophilic surface and improves the affinity of the SeN-Fe 3 C for CO 2. Density functional theory (DFT) calculations reveal that the electron-rich surface, which is caused by pyridinic N species and much more negatively charged Fe sites, leads to a high degree of polarization and activation of CO 2 molecule, thus conferring a remarkably improved CO 2 RR activity on the SeN-Fe 3 C catalyst. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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