dc.contributor.author | Chen, Wenyao | |
dc.contributor.author | Fu, Wenzhao | |
dc.contributor.author | Duan, Xuezhi | |
dc.contributor.author | Chen, Bingxu | |
dc.contributor.author | Qian, Gang | |
dc.contributor.author | Si, Rui | |
dc.contributor.author | Zhou, Xinggui | |
dc.contributor.author | Yuan, Weikang | |
dc.contributor.author | Chen, De | |
dc.date.accessioned | 2023-03-03T08:38:56Z | |
dc.date.available | 2023-03-03T08:38:56Z | |
dc.date.created | 2022-09-28T10:06:39Z | |
dc.date.issued | 2022 | |
dc.identifier.citation | Engineering (Beijing). 2022, 14 124-133. | en_US |
dc.identifier.issn | 2095-8099 | |
dc.identifier.uri | https://hdl.handle.net/11250/3055611 | |
dc.description.abstract | 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 relationships 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, contributing 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 manipulate metal–carbon catalysts with desirable properties. | en_US |
dc.language.iso | eng | en_US |
dc.publisher | Elsevier | en_US |
dc.rights | Attribution-NonCommercial-NoDerivatives 4.0 Internasjonal | * |
dc.rights.uri | http://creativecommons.org/licenses/by-nc-nd/4.0/deed.no | * |
dc.title | Taming Electrons in Pt/C Catalysts to Boost the Mesokinetics of Hydrogen Production | en_US |
dc.title.alternative | Taming Electrons in Pt/C Catalysts to Boost the Mesokinetics of Hydrogen Production | en_US |
dc.type | Peer reviewed | en_US |
dc.type | Journal article | en_US |
dc.description.version | publishedVersion | en_US |
dc.source.pagenumber | 124-133 | en_US |
dc.source.volume | 14 | en_US |
dc.source.journal | Engineering (Beijing) | en_US |
dc.identifier.doi | 10.1016/j.eng.2020.11.014 | |
dc.identifier.cristin | 2056203 | |
cristin.ispublished | true | |
cristin.fulltext | original | |
cristin.qualitycode | 1 | |