Optically and Electrocatalytically Decoupled Si Photocathodes with a Porous Carbon Nitride Catalyst for Nitrogen Reduction with Over 61.8% Faradaic Efficiency
© 2021 Wiley-VCH GmbH.
| Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 33(2021), 18 vom: 04. Mai, Seite e2100812 |
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| 1. Verfasser: | |
| Weitere Verfasser: | , , , , , , , |
| Format: | Online-Aufsatz |
| Sprache: | English |
| Veröffentlicht: |
2021
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| Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
| Schlagworte: | Journal Article decoupling light-harvesting and electrocatalysis nitrogen reduction photoelectrochemical porous carbon nitride |
| Zusammenfassung: | © 2021 Wiley-VCH GmbH. The photoelectrochemical (PEC) approach is attractive as a promising route for the nitrogen reduction reaction (NRR) toward ammonia (NH3 ) synthesis. However, the challenges in synergistic management of optical, electrical, and catalytic properties have limited the efficiency of PEC NRR devices. Herein, to enhance light-harvesting, carrier separation/transport, and the catalytic reactions, a concept of decoupling light-harvesting and electrocatalysis by employing a cascade n+ np+ -Si photocathode is implemented. Such a decoupling design not only abolishes the parasitic light blocking but also concurrently improves the optical and electrical properties of the n+ np+ -Si photocathode without compromising the efficiency. Experimental and density functional theory studies reveal that the porous architecture and N-vacancies promote N2 adsorption of the Au/porous carbon nitride (PCN) catalyst. Impressively, an n+ np+ -Si photocathode integrating the Au/PCN catalyst exhibits an outstanding PEC NRR performance with maximum Faradaic efficiency (FE) of 61.8% and NH3 production yield of 13.8 µg h-1 cm-2 at -0.10 V versus reversible hydrogen electrode (RHE), which is the highest FE at low applied potential ever reported for the PEC NRR |
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| Beschreibung: | Date Revised 05.05.2021 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202100812 |