首页|Rh/InGaN1-xOx nanoarchitecture for light-driven methane reforming with carbon dioxide toward syngas

Rh/InGaN1-xOx nanoarchitecture for light-driven methane reforming with carbon dioxide toward syngas

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Light-driven dry reforming of methane toward syngas presents a proper solution for alleviating climate change and for the sustainable supply of transportation fuels and chemicals.Herein,Rh/InGaN1-xOx nanowires supported by silicon wafer are explored as an ideal platform for loading Rh nanoparticles,thus assembling a new nanoarchitecture for this grand topic.In combination with the remarkable photo-thermal synergy,the O atoms in Rh/InGaN1-xOx can significantly lower the apparent activation energy of dry reforming of methane from 2.96 eV downward to 1.70 eV.The as-designed Rh/InGaN1-xOx NWs nanoarchitecture thus demonstrates a measurable syngas evolution rate of 180.9 mmol g-1cat h-1 with a marked selectivity of 96.3％under concentrated light illumination of 6 W cm-2.What is more,a high turnover number(TON)of 4182 mol syngas per mole Rh has been realized after six reuse cycles without obvious activity degradation.The correlative 18O isotope labeling experiments,in-situ irradiated X-ray photoelectron spectroscopy(1SI-XPS)and in-situ diffuse reflectance Fourier transform infrared spec-troscopy characterizations,as well as density functional theory calculations reveal that under light illu-mination,Rh/InGaN1-xOx NWs facilitate releasing *CH3 and H+from CH4 by holes,followed by H2 evolution from H+reduction with electrons.Subsequently,the O atoms in Rh/InGaN1-xOx can directly participate in CO generation by reacting with the *C species from CH4 dehydrogenation and contributes to the coke elimination,in concurrent formation of O vacancies.The resultant O vacancies are then replenished by CO2,showing an ideal chemical loop.This work presents a green strategy for syngas pro-duction via light-driven dry reforming of methane.

Dry reforming of methanePhoto-thermal catalysisRh/InGaN1-xOx nanowires

Yixin Li、Jinglin Li、Tianqi Yu、Liang Qiu、Syed M.Najib Hasan、Lin Yao、Hu Pan、Shamsul Arafin、Sharif Md.Sadaf、Lei Zhu、Baowen Zhou

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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,Shanghai 200240,China

Department of Electrical and Computer Engineering,The Ohio State University,Columbus,OH,43210,USA

China-UK Low Carbon College,Shanghai Jiao Tong University,Shanghai 201306,China

Centre Energie,Matériaux et Télécommunications,Institut National de la Recherche Scientifique(INRS)-Université du Quebec,Varennes J3X 1E4,Canada

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国家自然科学基金Oceanic Interdisciplinary Program of Shanghai Jiao Tong UniversityShanghai Pilot Program for Basic Research-Shanghai Jiao Tong University国家重点研发计划Shanghai Municipal Science and Technology Major Project加拿大自然科学与工程研究委员会项目Centre Energie,Matériaux et Télécommunications,Institut National de la Recherche Scientifique(INRS)-Université du Québec

22109095SL2022MS00721TQ14002072023YFB4004900RGPIN-2021-04250

2024

10.1016/j.scib.2024.02.020

科学通报(英文版)
中国科学院

科学通报(英文版)

CSTPCD
ISSN：1001-6538
年,卷(期)：2024.69(10)
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