摘要
Actual chemical states of single-atom metal on reducible supports remain a fiercely debated topic under reactive environments.Herein,we demonstrate that the single-atom Pt on Co_(3)O_(4)surface undergoes an in-situ reconstruction to form isolated Pt-Co bimetallic sites via reducing coordination number of Pt–O in the presence of hydrogen from both simulations and in-situ X-ray photoelectron spectroscopy.The modified chemical states of Pt greatly promoted H_(2)activation,thus delivering a significantly high turnover frequency of 7,448 h−1(19.5 times over Pt nanoparticles on Co_(3)O_(4))for hydrogenation of cinnamaldehyde.The satisfactory selectivity of 95.2%towards cinnamyl alcohol was ascribed to a tilted adsorption configuration of reactant on the catalyst surface via aldehyde group.We anticipate that the recognitions on in-situ reconstruction of single-atom catalysts(SACs)under the reducing conditions benefit the design of highly-performed hydrogenation catalysts.
基金
the National Natural Science Foundation of China(Nos.21872109 and 22002115)
S.Z.is also supported by the Guangdong Basic and Applied Basic Research Foundation(2022B1515020092)
the Fundamental Research Funds for the Central Universities(Nos.D5000210283,D5000210601,and D5000210829)。