Probing Ligand-Induced Cooperative Orbital Redistribution That Dominates Nanoscale Molecule-Surface Interactions with One-Unit-Thin TiO2 Nanosheets

doi:10.1021/acs.nanolett.8b03572

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	Probing Ligand-Induced Cooperative Orbital Redistribution That Dominates Nanoscale Molecule-Surface Interactions with One-Unit-Thin TiO2 Nanosheets
	Xiang, Guolei; Tang, Yan; Zhu, Wei; Liu, Haitao; Wang, Jiaou; Zhong, Guiming; Wang JO(王嘉鸥); Li, Jun; Liu, Zigeng; Wang, Xun
刊名	NANO LETTERS
	2018
卷号	18 期号:12 页码:7809-7815
关键词	Nanosurface science coverage effect nanoscale cooperative chemisorption TiO2 nanosheet NEXAFS
ISSN号	1530-6984
DOI	10.1021/acs.nanolett.8b03572
文献子类	Article
英文摘要	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.
电子版国际标准刊号	1530-6992
WOS关键词	ELECTRONIC-STRUCTURE ; GOLD ; CATALYSIS ; CONFINEMENT ; REACTIVITY ; CLUSTERS ; SCIENCE
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
语种	英语
WOS记录号	WOS:000453488800051
内容类型	期刊论文
源URL	[http://ir.ihep.ac.cn/handle/311005/286869]
专题	中国科学院高能物理研究所_中国散裂中子源高能物理研究所_多学科研究中心高能物理研究所_东莞分部
作者单位	中国科学院高能物理研究所
推荐引用方式 GB/T 7714	Xiang, Guolei,Tang, Yan,Zhu, Wei,et al. Probing Ligand-Induced Cooperative Orbital Redistribution That Dominates Nanoscale Molecule-Surface Interactions with One-Unit-Thin TiO2 Nanosheets[J]. NANO LETTERS,2018,18(12):7809-7815.
APA	Xiang, Guolei.,Tang, Yan.,Zhu, Wei.,Liu, Haitao.,Wang, Jiaou.,...&Wang, Xun.(2018).Probing Ligand-Induced Cooperative Orbital Redistribution That Dominates Nanoscale Molecule-Surface Interactions with One-Unit-Thin TiO2 Nanosheets.NANO LETTERS,18(12),7809-7815.
MLA	Xiang, Guolei,et al."Probing Ligand-Induced Cooperative Orbital Redistribution That Dominates Nanoscale Molecule-Surface Interactions with One-Unit-Thin TiO2 Nanosheets".NANO LETTERS 18.12(2018):7809-7815.