首页|Triple the steady-state reaction rate by decorating the In2O3 surface with SiOx for CO2 hydrogenation

Triple the steady-state reaction rate by decorating the In2O3 surface with SiOx for CO2 hydrogenation

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Indium oxide(In2O3),as a promising candidate for CO2 hydrogenation to C1 products,often suffers from sintering and activity decline,closely related to the undesirable structural evolution under reaction con-ditions.Based on the comprehension of the dynamic evolution,this study presents an efficient strategy to alleviate the agglomeration of In2O3 nanoparticles by the surface decoration with highly dispersed silica species(SiOx).Various structural characterizations combined with density functional theory calculations demonstrated that the sintering resulted from the over-reduction,while the enhanced stability origi-nated from the anchoring effect of highly stable In-OSi bonds,which hinders the substantial formation of metallic In(In0)and the subsequent agglomeration.0.6Si/In2O3 exhibited CO2 conversion rate of 10.0 mmol g-1 h-1 at steady state vs.3.5 mmol g-1 h-1 on In2O3 in CO2 hydrogenation.Enhanced steady-state activity was also achieved on Pd-modified catalysts.Compared to the traditional Pd/In2O3 catalyst,the methanol production rate of Pd catalyst supported on 0.6Si/In2O3 was enhanced by 23％,showing the potential of In2O3 modified by SiOx in serving as a platform material.This work provides a promising method to design new In2O3-based catalysts with improved activity and stability in CO2 hydrogenation.

CO2 hydrogenationIn2O3 sinteringDynamic structural evolutionSurface SiOx modificationDFT simulations

Hao Wang、Chun Yang、Xiaoyan Yu、Mingrui Wang、Runze Yang、Xiaowa Nie、Ben Hang Yin、Alex C.K.Yip、Chunshan Song、Guanghui Zhang、Xinwen Guo

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State Key Laboratory of Fine Chemicals,Frontier Science Center for Smart Materials,PSU-DUT Joint Center for Energy Research,School of Chemical Engineering,Dalian University of Technology,Dalian 116024,Liaoning,China

Paihau-Robinson Research Institute,the MacDiarmid Institute for Advanced Materials and Nanotechnology,Victoria University of Wellington,Wellington 6012,New Zealand

Department of Chemical and Process Engineering,The University of Canterbury,Christchurch 8041,New Zealand

Department of Chemistry,the Chinese University of Hong Kong,Hong Kong 999077,China

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National Natural Science Foundation of ChinaSpecial Project for Key Research and Development Program of Xinjiang Autonomous RegionLiaoning Revitalization Talent ProgramLiaoning Revitalization Talent ProgramFundamental Research Funds for the Central UniversitiesFundamental Research Funds for the Central UniversitiesFundamental Research Funds for the Central UniversitiesCUHK Research Startup FundCatalyst:Seeding fundingNew Zealand Ministry of Business,Innovation and EmploymentRoyal Society Apārangi

221720132022B01033-3XLYC2008032XLYC2203126DUT22LK24DUT22QN207DUT22LAB6024930981CSG-VUW2201

2024

10.1016/j.jechem.2024.03.041

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.95(8)