The dynamic and kinetic evolution of supported metal particles in the presence of reactants is decisive in shaping the nature of the catalytic active sites and the deactivation process. Ostwald ripening of FeO/Pt(111)...The dynamic and kinetic evolution of supported metal particles in the presence of reactants is decisive in shaping the nature of the catalytic active sites and the deactivation process. Ostwald ripening of FeO/Pt(111) supported Au particles in the presence of carbon monoxide is addressed here by firstprinciples kinetics. It is found that CO stabilizes the ripening monomer(Au atom) by forming favorable Au carbonyls with lower total activation energy, and corresponding phase diagram at wide range of temperature and CO pressures is constructed. Evolution of particle number, dispersion and particle size distribution of supported Au particles are explored. Great influence of CO promotion on ripening kinetics is revealed and explored in details, and mbar range of CO can lower the onset temperature of ripening by a few hundred kelvins. The present work reveals the crucial role of the metal-reactant complexes formed under reaction conditions on ripening of metal catalysts.展开更多
基金supported by the National Key R&D Program of China(2021YFB3502000,2018YFA0208603)National Program for Support of Top-notch Young Professional,Chinese Academy of Sciences Youth Innovation Promotion Association,Anhui Outstanding Youth Fund(No.2208085J27)+6 种基金the National Natural Science Foundation of China(No.22221003,No.91945302,No.21903077)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0450102)Innovation Program for Quantum Science and Technology(2021ZD0303302)Chinese Academy of Sciences(QYZDJ-SSW-SLH054)K.C.Wong Education(GJTD-2020-15)the Dalian National Laboratory For Clean Energy(DNL)Cooperation Fund,the CAS(DNL201920)the China Postdoctoral Science Foundation,the Fundamental Research Funds for the Central Universities,USTC Research Funds of the Double First-Class Initiative(KY9990000170,YD9990002008)。
基金supported by the National Key R&D Program of China(2017YB0602205)the National Natural Science Foundation of China(91645202)the Chinese Academy of Sciences(QYZDJSSW-SLH054)
文摘The dynamic and kinetic evolution of supported metal particles in the presence of reactants is decisive in shaping the nature of the catalytic active sites and the deactivation process. Ostwald ripening of FeO/Pt(111) supported Au particles in the presence of carbon monoxide is addressed here by firstprinciples kinetics. It is found that CO stabilizes the ripening monomer(Au atom) by forming favorable Au carbonyls with lower total activation energy, and corresponding phase diagram at wide range of temperature and CO pressures is constructed. Evolution of particle number, dispersion and particle size distribution of supported Au particles are explored. Great influence of CO promotion on ripening kinetics is revealed and explored in details, and mbar range of CO can lower the onset temperature of ripening by a few hundred kelvins. The present work reveals the crucial role of the metal-reactant complexes formed under reaction conditions on ripening of metal catalysts.
基金supported by the National Natural Science Foundation of China(21978283,22090060,and 22090063)the Strategic Priority Research Program of Chinese Academy of Sciences(XDB17020400)+4 种基金Liaoning Revitalization Talents Program(XLYC1801004)the DNL Cooperation Fund,Chinese Academy of Sciences(DNL201920)Youth Innovation Promotion Association of Chinese Academy of Sciences,and Dalian Institute of Chemical Physics(DICP ZZBS201711)the financial support of National Key R&D Program of China(2018YFA0208603)K.C.Wong Education Foundation(GJTD-2020-15)。
