Optically and Electrocatalytically Decoupled Si Photocathodes with a Porous Carbon Nitride Catalyst for Nitrogen Reduction with Over 61.8% Faradaic Efficiency.

Autor: Peramaiah K; KAUST Catalysis Center, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.; Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.; Division of Computer, Electrical and Mathematical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia., Ramalingam V; KAUST Catalysis Center, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.; Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.; Division of Computer, Electrical and Mathematical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia., Fu HC; Division of Computer, Electrical and Mathematical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia., Alsabban MM; KAUST Catalysis Center, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.; Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.; Department of Chemistry, University of Jeddah, Jeddah, 21959, Kingdom of Saudi Arabia., Ahmad R; KAUST Catalysis Center, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.; Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia., Cavallo L; KAUST Catalysis Center, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.; Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia., Tung V; KAUST Catalysis Center, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.; Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia., Huang KW; KAUST Catalysis Center, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.; Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia., He JH; KAUST Catalysis Center, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.; Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, SAR 999077, Hong Kong.
Jazyk: angličtina
Zdroj: Advanced materials (Deerfield Beach, Fla.) [Adv Mater] 2021 May; Vol. 33 (18), pp. e2100812. Date of Electronic Publication: 2021 Mar 31.
DOI: 10.1002/adma.202100812
Abstrakt: The photoelectrochemical (PEC) approach is attractive as a promising route for the nitrogen reduction reaction (NRR) toward ammonia (NH 3 ) 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 N 2 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 NH 3 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.
(© 2021 Wiley-VCH GmbH.)
Databáze: MEDLINE
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