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光驱动Rh/InGaN_(1-x)O_(x)纳米组装体甲烷干重整制合成气

Science Bulletin 2024年第10期69卷 1400-1409页

作者：李亦昕李景林俞天奇邱亮 Syed M.Najib Hasan 姚琳潘虎 shamsul arafin Sharif Md.Sadaf 朱磊周宝文 Key Laboratory for Power Machinery and Engineering of Ministry of Education Research Center for Renewable Synthetic FuelSchool of Mechanical EngineeringShanghai Jiao Tong UniversityShanghai 200240China China-UK Low Carbon College Shanghai Jiao Tong UniversityShanghai 201306China Centre Energie Matériaux et TélécommunicationsInstitut National de la Recherche Scientifique(INRS)-Universitédu QuébecVarennes J3X 1E4Canada Department of Electrical and Computer Engineering The Ohio State UniversityColumbusOH43210USA

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 ***,Rh/InGaN_(1-x)O_(x) nanowires supported by silicon wafer are explored as an ideal platform for loading Rh nanoparticles,thus assembling a new nanoarchitecture for this grand *** combination with the remarkable photothermal synergy,the O atoms in Rh/InGaN_(1-x)O_(x) can significantly lower the apparent activation energy of dry reforming of methane from 2.96 eV downward to 1.70 *** as-designed Rh/InGaN_(1-x)O_(x) NWs nanoarchitecture thus demonstrates a measurable syngas evolution rate of 180.9 mmol g_(cat)^(-1) 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 *** correlative 18O isotope labeling experiments,in-situ irradiated X-ray photoelectron spectroscopy(ISI-XPS)and in-situ diffuse reflectance Fourier transform infrared spectroscopy characterizations,as well as density functional theory calculations reveal that under light illumination,Rh/InGaN_(1-x)O_(x) NWs facilitate releasing^(*)CH_(3) and H^(+)from CH_(4) by holes,followed by H_(2) evolution from H^(+)reduction with ***,the O atoms in Rh/InGaN_(1-x)O_(x) can directly participate in CO generation by reacting with the ^(*)C species from CH_(4) dehydrogenation and contributes to the coke elimination,in concurrent formation of O *** resultant O vacancies are then replenished by CO_(2),showing an ideal chemical *** work presents a green strategy for syngas production via light-driven dry reforming of methane.

关键词： Dry reforming of methane Photo-thermal catalysis Rh/InGaN_(1-x)O_(x)nanowires

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