A semiconducting hybrid of RhO x /GaN@InGaN for simultaneous activation of methane and water toward syngas by photocatalysis.

Autor: Li D; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China.; School of Physics, Liaoning University, No. 66 Chongshan Middle Road, Huanggu District, Shenyang City 110036, Liaoning Province, China., Wu Z; College of Physics and Optoelectronic Engineering, Shenzhen University, 3688 Nanhai Avenue, Nanshan District, Shenzhen 518061, China., Li Y; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China., Fan X; School of Physics, Liaoning University, No. 66 Chongshan Middle Road, Huanggu District, Shenyang City 110036, Liaoning Province, China., Hasan SMN; Electrical and Computer Engineering, The Ohio State University, Columbus, OH 43210, USA., Arafin S; Electrical and Computer Engineering, The Ohio State University, Columbus, OH 43210, USA., Rahman MA; Centre Energie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique (INRS)-Université du Québec, 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X1S2, Canada., Li J; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China., Wang Z; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China., Yu T; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China., Kong X; College of Physics and Optoelectronic Engineering, Shenzhen University, 3688 Nanhai Avenue, Nanshan District, Shenzhen 518061, China., Zhu L; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China., Sadaf SM; Centre Energie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique (INRS)-Université du Québec, 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X1S2, Canada., Zhou B; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China.
Jazyk: angličtina
Zdroj: PNAS nexus [PNAS Nexus] 2023 Nov 21; Vol. 2 (11), pp. pgad347. Date of Electronic Publication: 2023 Nov 21 (Print Publication: 2023).
DOI: 10.1093/pnasnexus/pgad347
Abstrakt: Prior to the eventual arrival of carbon neutrality, solar-driven syngas production from methane steam reforming presents a promising approach to produce transportation fuels and chemicals. Simultaneous activation of the two reactants, i.e. methane and water, with notable geometric and polar discrepancy is at the crux of this important subject yet greatly challenging. This work explores an exceptional semiconducting hybrid of RhO x /GaN@InGaN nanowires for overcoming this critical challenge to achieve efficient syngas generation from methane steam reforming by photocatalysis. By coordinating density functional theoretical calculations and microscopic characterizations, with in situ spectroscopic measurements, it is found that the multifunctional RhO x /GaN interface is effective for simultaneously activating both CH 4 and H 2 O by stretching the C-H and O-H bonds because of its unique Lewis acid/base attribute. With the aid of energetic charge carriers, the stretched C-H and O-H bonds of reactants are favorably cleaved, resulting in the key intermediates, i.e. *CH 3 , *OH, and *H, to sit on Rh sites, Rh sites, and N sites, respectively. Syngas is subsequently produced via energetically favored pathway without additional energy inputs except for light. As a result, a benchmarking syngas formation rate of 8.1 mol·g cat -1 ·h -1 is achieved with varied H 2 /CO ratios from 2.4 to 0.8 under concentrated light illumination of 6.3 W·cm -2 , enabling the achievement of a superior turnover number of 10,493 mol syngas per mol Rh species over 300 min of long-term operation. This work presents a promising strategy for green syngas production from methane steam reforming by utilizing unlimited solar energy.
(© The Author(s) 2023. Published by Oxford University Press on behalf of National Academy of Sciences.)
Databáze: MEDLINE
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