Taming the electron transfer across metal–support interfaces appears to be an attractive yet challenging methodology to boost catalytic properties. Herein, we demonstrate a precise engineering strategy for the carbon surface chemistry of Pt/C catalysts—that is, for the electron-withdrawing/donating oxygen-containing groups on the carbon surface—to fine-tune the electrons of the supported metal nanoparticles. Taking the ammonia borane hydrolysis as an example, a combination of density functional theory (DFT) calculations, advanced characterizations, and kinetics and isotopic analyses reveals quantifiable relation-ships among the carbon surface chemistry, Pt charge state and binding energy, activation entropy/enthalpy, and resultant catalytic activity. After decoupling the influences of other factors, the Pt charge is unprecedentedly identified as an experimentally measurable descriptor of the Pt active site, contribut-ing to a 15-fold increment in the hydrogen generation rate. Further incorporating the Pt charge with the number of Pt active sites, a mesokinetics model is proposed for the first time that can individually quantify the contributions of the electronic and geometric properties to precisely predict the catalytic performance. Our results demonstrate a potentially groundbreaking methodology to design and manip-ulate metal–carbon catalysts with desirable properties.

Wenyao Chen;Wenzhao Fu;Xuezhi Duan;Bingxu Chen;Gang Qian;Rui Si;Xinggui Zhou;Weikang Yuan;De Chen

State Key Laboratory of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China;Shanghai Synchrotron Radiation Facility,Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai 201204,China;Department of Chemical Engineering,Norwegian University of Science and Technology,Trondheim N-7491,Norway

工程（英文）

[1]Wenyao Chen;Wenzhao Fu;Xuezhi Duan;Bingxu Chen;Gang Qian;Rui Si;Xinggui Zhou;Weikang Yuan;De Chen-.Taming Electrons in Pt/C Catalysts to Boost the Mesokinetics of Hydrogen Production)[J].工程（英文）,2022(07):124-133

Taming,Mesokinetics,contribut,mesokinetics

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