期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 11, 页码 3527-3532出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201813958
关键词
adsorption; hydrogen; hydrogen binding energy; platinum; water phase
资金
- 111Project of China [B17020]
- postdoctoral international exchange program of China
- Chemical Transformation Initiative at Pacific Northwest National Laboratory (PNNL)
- United States Department of Energy (U.S. DOE), the Bioenergy Technologies Office
- [DE-AC02-05CH11231]
The thermodynamic state of H-2 adsorbed on Pt in the aqueous phase was determined by kinetic analysis of H-2 reacting with D2O to HDO, HD, and D-2, and by DFT-based ab initio molecular dynamics simulations of H-2 adsorption on Pt(111), Pt(110), and Pt nanoparticles. Dissociative adsorption of H-2 on Pt is significantly weakened in the aqueous phase compared to adsorption at gas-solid interfaces. Water destabilizes the adsorbed H atoms, decreasing the heat of adsorption by 19-22 kJ molH2-1 while inducing an additional entropy loss of 50-70 J molH2-1 K-1. Upon dissociative adsorption of H-2, the average distance of water from the Pt surface increases and the liquid adopts a structure that is more ordered than before close to the Pt surface, which limits the translation mobility of the adsorbed H atoms. The presence of hydrated hydronium ions next to the Pt surface further lowers the H-Pt bond strength.
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