Zeolitic imidazole framework-derived FeN5-doped carbon as superior CO2 electrocatalysts
| Autor: | Huiyuan Cheng, Zihao Fan, Yayun Zhang, Xuemei Wu, Xiangcun Li, Manman Feng, Gaohong He |
|---|---|
| Rok vydání: | 2021 |
| Předmět: |
010405 organic chemistry
Doped carbon Multiple applications 010402 general chemistry Electrochemistry 01 natural sciences Combinatorial chemistry Catalysis 0104 chemical sciences chemistry.chemical_compound chemistry Pyridine Imidazole Density functional theory Physical and Theoretical Chemistry Faraday efficiency |
| Zdroj: | Journal of Catalysis. 395:63-69 |
| ISSN: | 0021-9517 |
| DOI: | 10.1016/j.jcat.2020.12.032 |
| Popis: | Electrochemical CO2 conversion offers a sustainable approach to alleviate the energy crisis but remains a long-standing challenge. Herein, atomically dispersed FeN5 sites anchored on N-doped carbon matrix templated by zeolitic imidazole framework-8 (ZIF-8) are facilely synthesized for efficient catalyzing CO2 reduction. The FeN5 single-atom catalyst (Fe-SA/ZIF) presents the Faradaic efficiency of 98% at −0.7 V vs. RHE and over 95% in a wide potential range from −0.4 to −1.0 V vs. RHE, surpassing most of the reported single-atom catalysts for CO2RR. Further density functional theory (DFT) calculations reveal that the outstanding activity of FeN5 sites mainly originates from the lowered d-band center modulated by the out-of-plane coordinated pyridinic N, which reduces the CO adsorption energy from −1.71 to −1.49 eV compared to FeN4 moieties. Thus, the synergistic effect between FeN4 sites and the coordinated pyridine offers new insight in designing outstanding electrocatalysts for multiple applications. |
| Databáze: | OpenAIRE |
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