期刊
JOURNAL OF PHYSICS-CONDENSED MATTER
卷 33, 期 24, 页码 -出版社
IOP Publishing Ltd
DOI: 10.1088/1361-648X/abe9da
关键词
first-principle calculation; basal plane; hydrogen evolution reaction; electrocatalysts; 2D catalysts
资金
- National Natural Science Foundation of China [11504086]
- Ten Thousand Talents Plan of Zhejiang Province of China [2019R52014]
- Open Project of National Laboratory of Solid State Microstructures, Nanjing University [M33010]
- School Scientific Research Project of Hangzhou Dianzi University [KYS045619084, KYS045619085]
The study found that on a single-atom-anchored 2D basal plane, hydrogen adsorption mainly occurs through the hybridization between the 1s orbital of H and the vertical d(z2) orbital of anchored atoms, with a linear relation between the d(z2)-band center and H bond strength, serving as an activity descriptor for the hydrogen evolution reaction.
The d-band center descriptor based on the adsorption strength of adsorbate has been widely used in understanding and predicting the catalytic activity in various metal catalysts. However, its applicability is unsure for the single-atom-anchored two-dimensional (2D) catalysts. Here, taking the hydrogen (H) adsorption on the single-atom-anchored 2D basal plane as example, we examine the influence of orbitals interaction on the bond strength of hydrogen adsorption. We find that the adsorption of H is formed mainly via the hybridization between the 1s orbital of H and the vertical d(z2) orbital of anchored atoms. The other four projected d orbitals (d(xy)/d(x2-y2), d(xz)/d(yz)) have no contribution to the H chemical bond. There is an explicit linear relation between the d(z2)-band center and the H bond strength. The d(z2)-band center is proposed as an activity descriptor for hydrogen evolution reaction (HER). We demonstrate that the d(z2)-band center is valid for the single-atom active sites on a single facet, such as the basal plane of 2D nanosheets. For the surface with multiple facets, such as the surface of three-dimensional (3D) polyhedral nanoparticles, the d-band center is more suitable.
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