https://scholars.lib.ntu.edu.tw/handle/123456789/606871
標題: | Unveiling the in Situ Generation of a Monovalent Fe(I) Site in the Single-Fe-Atom Catalyst for Electrochemical CO2 Reduction | 作者: | Li X Zeng Y Tung C.-W Lu Y.-R Baskaran S Hung S.-F Wang S Xu C.-Q Wang J Chan T.-S Chen H.M Jiang J Yu Q Huang Y Li J Zhang T Liu B. HAO MING CHEN |
關鍵字: | electrochemistry;M?ssbauer spectroscopy;operando;reaction mechanism;single-atom catalyst;Atoms;Carbon dioxide;Density functional theory;Electrocatalysts;Iron metallography;Spectroscopic analysis;X ray absorption spectroscopy;CO2 reduction;Coordination environment;Optimal binding;Orbital interaction;Pyrrolic nitrogen;Single atoms;Situ generation;Spectroscopic studies;Iron compounds | 公開日期: | 2021 | 卷: | 11 | 期: | 12 | 起(迄)頁: | 7292-7301 | 來源出版物: | ACS Catalysis | 摘要: | Atomically dispersed single-atom catalysts are among the most attractive electrocatalysts for the CO2 reduction reaction (CRR). To elucidate the origin of the exceptional activity of atomically dispersed Fe-N-C catalyst in CRR, we have performed operando 57Fe M?ssbauer spectroscopic studies on a model single-Fe-atom catalyst with a well-defined N coordination environment. Combining with operando X-ray absorption spectroscopy, the in situ-generated four pyrrolic nitrogen atom-coordinated low-spin Fe(I) (LS FeIN4) featuring monovalent iron is identified as the reactive center for the conversion of CO2 to CO. Furthermore, density functional theory calculations reveal that the optimal binding strength of CO2 to the LS FeIN4 site, with strong orbital interactions between the singly occupied dz2 orbital of the Fe(I) site and the singly occupied π? orbital of [COOH] fragment, is the key factor for the excellent CRR performance. ? 2021 American Chemical Society. |
URI: | https://www.scopus.com/inward/record.uri?eid=2-s2.0-85108646100&doi=10.1021%2facscatal.1c01621&partnerID=40&md5=a5fdc485e1d52aefa236a36ad5589712 https://scholars.lib.ntu.edu.tw/handle/123456789/606871 |
ISSN: | 21555435 | DOI: | 10.1021/acscatal.1c01621 |
顯示於: | 化學系 |
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