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Visible light-enhanced photothermal CO2 hydrogenation over Pt/Al2O3 catalyst

Chinese Journal of Catalysis 2020年第2期41卷 286-293页

作者： Ziyan Zhao Dmitry EDoronkin Yinghao Ye jan-dierk grunwaldt Zeai Huang Ying Zhou State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation Southwest Petroleum UniversityChengdu 610500SichuanChina The Center of New Energy Materials and Technology School of Materials Science and EngineeringSouthwest Petroleum UniversityChengdu 610500SichuanChina Institute for Chemical Technology and Polymer Chemistry(ITCP) Karlsruhe Institute of TechnologyKarlsruhe(KIT)76131 KarlsruheGermany Institute of Catalysis Research and Technology(IKFT) Karlsruhe Institute of Technology(KIT)76344 Eggenstein-LeopoldshafenGermany

Light illumination has been widely used to promote activity and selectivity of traditional thermal catalysts. Nevertheless, the role of light irradiation during catalytic reactions is not well understood. In this work, Pt/Al2 O3 prepared by wet impregnation was used for photothermal CO2 hydrogenation, and it showed a photothermal effect. Hence, operando diffuse reflectance infrared Fourier-transform spectroscopy and density functional theory calculations were conducted on Pt/Al2 O3 to gain insights into the reaction mechanism. The results indicated that CO desorption from Pt sites including step sites(Ptstep) or/and terrace site(Ptterrace) is an important step during CO2 hydrogenation to free the active Pt sites. Notably, visible light illumination and temperature affected the CO desorption in different ways. The calculated adsorption energy of CO on Ptstep and Ptterrace sites was-1.24 and-1.43 e V, respectively. Hence, CO is more strongly bound to the Ptstep sites. During heating in the dark, CO preferentially desorbs from the Ptterrace site. However, the additional light irradiation facilitates transfer of CO from the Ptstep to Ptterrace sites and its subsequent desorption from the Ptterrace sites, thus promoting the CO2 hydrogenation.

关键词： CO2 hydrogenation Photothermal catalysis Pt/Al2O3 Operando diffuse reflectance infrared Fourier transform spectroscopy Density functional theory

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Reduction and carburization of iron oxides for Fischer–Tropsch synthesis

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Journal of Energy Chemistry 2020年第12期29卷 48-61页

作者： Monia Runge Nielsen Asger Barkholt Moss Anton Simon Bjrnlund Xi Liu Axel Knop-Gericke Alexander YuKlyushin jan-dierk grunwaldt Thomas LSheppard Dmitry EDoronkin Anna Zimina Thomas Eric Lyck Smitshuysen Christian Danvad Damsgaard Jakob Birkedal Wagner Thomas Willum Hansen DTU Nanolab Technical University of DenmarkDK-2800Kgs.LyngbyDenmark Department of Physics Technical University of DenmarkDK-2800Kgs.LyngbyDenmark SynCat@Beijing Synfuels China Technology Co.LtdBeijing 101407China School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China Department of Inorganic Chemistry Fritz Haber Institute of the Max Planck SocietyD-14195 BerlinGermany Research Group Heterogeneous Reactions.Max Planck Institute for Chemical Energy Conversion D-45470 MulheimGermany Research Group Catalysis for Energy Helmholtz-Zentrum Berlin for Materials and Energy(BESSYⅡ)D-12489 BerlinGermany Institute for Chemical Technology and Polymer Chemistry Karlsruhe Institute of TechnologyD-76131 KarlsruheGermany Institute of Catalysis Research and Technology Karlsruhe Institute of TechnologyD-76344 Eggenstein-LeopoldshafenGermany

The activation of iron oxide Fischer–Tropsch Synthesis(FTS) catalysts was investigated during pretreatment: reduction in hydrogen followed by carburization in either CO or syngas mixture, or simultaneously reduction and carburization in syngas. A combination of different complementary in situ techniques was used to gain insight into the behavior of Fe-based FTS catalysts during activation. In situ XRD was used to identify the crystalline structures present during both reduction in hydrogen and carburization. An increase in reduction rate was established when increasing the temperature. A complete reduction was demonstrated in the ETEM and a grain size dependency was proven, i.e. bigger grains need higher temperature in order to reduce. XPS and XAS both indicate the formation of a small amount of carbonaceous species at the surface of the bulk metallic iron during carburization.

关键词： In situ characterization Fischer–Tropsch Catalyst reduction and carburization Iron oxides

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