In the field of noble metal-catalyzed alcohol electro-oxidation reaction(AOR),huge attention is paid on the composition,size,facet,and structure of the metals,while the support engineering should also be emphasized.Ce...In the field of noble metal-catalyzed alcohol electro-oxidation reaction(AOR),huge attention is paid on the composition,size,facet,and structure of the metals,while the support engineering should also be emphasized.CeO_(2)has been widely used as a unique support in AOR,primarily due to its abundant oxygen vacancies(O_(v)).Herein,we report CeO_(2)·xH_(2)O nanoparticles with both massive hydroxyl groups(OH)and O_(v)remarkably enhance the catalytic activity and stability of Pd toward ethanol oxidation reaction(EOR).The CO striping experiments and density functional theory(DFT)calculations suggest that OH and O_(v)on CeO_(2)·xH_(2)O surface bring about a large downshift of Pd d-band center and a significant weakening of CO absorption on Pd.Moreover,OH and O_(v)also play synergic roles in the removal of toxic intermediates.Consequently,the important roles of OH and O_(v)of CeO_(2)·xH_(2)O are confirmed in Pd-catalyzed EOR.The facile CeO_(2)·xH_(2)O-enhanced strategy can contribute to the catalyst design for other energy conversion reactions.展开更多
基金supported by the National Natural Science Foundation of China(21875125,22161033)the 111 Project(D20033)+2 种基金the Natural Science Foundation of Inner Mongolia Autonomous Region of China(2017JQ03)“Grassland Talent”Program“Grassland Talent”Innovation Team of Inner Mongolia。
文摘In the field of noble metal-catalyzed alcohol electro-oxidation reaction(AOR),huge attention is paid on the composition,size,facet,and structure of the metals,while the support engineering should also be emphasized.CeO_(2)has been widely used as a unique support in AOR,primarily due to its abundant oxygen vacancies(O_(v)).Herein,we report CeO_(2)·xH_(2)O nanoparticles with both massive hydroxyl groups(OH)and O_(v)remarkably enhance the catalytic activity and stability of Pd toward ethanol oxidation reaction(EOR).The CO striping experiments and density functional theory(DFT)calculations suggest that OH and O_(v)on CeO_(2)·xH_(2)O surface bring about a large downshift of Pd d-band center and a significant weakening of CO absorption on Pd.Moreover,OH and O_(v)also play synergic roles in the removal of toxic intermediates.Consequently,the important roles of OH and O_(v)of CeO_(2)·xH_(2)O are confirmed in Pd-catalyzed EOR.The facile CeO_(2)·xH_(2)O-enhanced strategy can contribute to the catalyst design for other energy conversion reactions.
