Potassium-Assisted Fabrication of Intrinsic Defects in Porous Carbons for Electrocatalytic CO2 Reduction
© 2022 Wiley-VCH GmbH.
| Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 34(2022), 42 vom: 23. Okt., Seite e2205933 |
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| 1. Verfasser: | |
| Weitere Verfasser: | , , , , , , , |
| Format: | Online-Aufsatz |
| Sprache: | English |
| Veröffentlicht: |
2022
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| Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
| Schlagworte: | Journal Article CO2 conversion defects electrocatalysis metal-organic frameworks porous carbon |
| Zusammenfassung: | © 2022 Wiley-VCH GmbH. The fabrication of intrinsic carbon defects is usually tangled with doping effects, and the identification of their unique roles in catalysis remains a tough task. Herein, a K+ -assisted synthetic strategy is developed to afford porous carbon (K-defect-C) with abundant intrinsic defects and complete elimination of heteroatom via direct pyrolysis of K+ -confined metal-organic frameworks (MOFs). Positron-annihilation lifetime spectroscopy, X-ray absorption fine structure measurement, and scanning transmission electron microscopy jointly illustrate the existence of abundant 12-vacancy-type carbon defects (V12 ) in K-defect-C. Remarkably, the K-defect-C achieves ultrahigh CO Faradaic efficiency (99%) at -0.45 V in CO2 electroreduction, far surpassing MOF-derived carbon without K+ etching. Theoretical calculations reveal that the V12 defects in K-defect-C favor CO2 adsorption and significantly accelerate the formation of the rate-determining COOH* intermediate, thereby promoting CO2 reduction. This work develops a novel strategy to generate intrinsic carbon defects and provides new insights into their critical role in catalysis |
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| Beschreibung: | Date Revised 20.10.2022 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202205933 |