期刊
NANO LETTERS
卷 18, 期 12, 页码 7809-7815出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.8b03572
关键词
Nanosurface science; coverage effect; nanoscale cooperative chemisorption; TiO2 nanosheet; NEXAFS
类别
资金
- Fundamental Research Funds for Central Universities of China [buctrc201812]
- National Natural Science Foundation of China [21431003, 21521091, 21590792, 91645203, 21801012]
- Public Hatching Platform for Recruited Talents of Beijing University of Chemical Technology
Understanding the general electronic principles underlying molecule surface interactions at the nanoscale is crucial for revealing the processes based on chemisorption, like catalysis, surface ligation, surface fluorescence, etc. However, the electronic mechanisms of how surface states affect and even dominate the properties of nanomaterials have long remained unclear. Here, using one-unit-thin TiO2 nanosheet as a model surface platform, we find that surface ligands can competitively polarize and confine the valence 3d orbitals of surface Ti atoms from delocalized energy band states to localized chemisorption bonds, through probing the surface chemical interaction at the orbital level with near-edge X-ray absorption fine structure (NEXAFS). Such ligand-induced orbital redistributions, which are revealed by combining experimental discoveries, quantum calculations, and theoretical analysis, are cooperative with ligand coverages and can enhance the strength of chemisorption and ligation-induced surface effects on nanomaterials. The model and concept of nanoscale cooperative chemisorption reveal the general physical principle that drives the coverage-dependent ligand-induced surface effects on regulating the electronic structures, surface activity, optical properties, and chemisorption strength of nanomaterials.
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