Structural and Optical Interplay of Palladium-Modified TiO 2 Nanoheterostructure
Abstract
The electronic structure and optical properties of Pd-modified TiO2 nanotubes (NTs) with a vertically aligned nanotubular structure grown by a two-step electrochemical anodization method have been studied using X-ray spectroscopy. X-ray absorption near-edge structure (XANES) at the Ti L3,2- and O K-edges was used to investigate the TiO2 NTs before and after Pd modification. It was found that Pd nanoparticles (NPs) are uniformly coated on the NT surface. The Pd L3-edge of the deposited Pd NPs shows a more intense whiteline and a blue shift for the Pd L3-edge absorption threshold relative to Pd metal, indicating charge depletion from the Pd 4d orbital as a result NP formation. The lattice of Pd is slightly contracted upon NP formation, although it remains fcc as revealed by extended X-ray absorption fine structure (EXAFS) analysis at the Pd K-edge. X-ray-excited optical luminescence (XEOL) together with XANES with element and site specificity was used to study the optical luminescence from TiO2 NTs. It was found that the defect-originated XEOL intensity dropped noticeably in the Pd NP-coated NTs, suggesting a Pd NP–TiO2-interaction-mediated reduction in the radiative recombination of electrons and holes. Finally, further evidence is provided by Ti 2p resonant inelastic X-ray scattering (RIXS), inmore »
- Authors:
-
- Department of Chemistry, University of Western Ontario, 1151 Richmond Street, London, Ontario N6A5B7, Canada
- Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States; National Synchrotron Radiation Laboratory and Collaborative Innovation Center of Suzhou Nano Science and Technology, University of Science and Technology of China, Hefei, Anhui 230029, People’s Republic of China
- National Synchrotron Radiation Laboratory and Collaborative Innovation Center of Suzhou Nano Science and Technology, University of Science and Technology of China, Hefei, Anhui 230029, People’s Republic of China
- Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1512161
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 119; Journal Issue: 4; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electronic structure; X-ray absorption near edge structure; extended X-ray absorption fine structure; X-ray excited optical luminescence; resonant inelastic X-ray scattering
Citation Formats
Li, Jun, Sham, Tsun-Kong, Ye, Yifan, Zhu, Junfa, and Guo, Jinghua. Structural and Optical Interplay of Palladium-Modified TiO 2 Nanoheterostructure. United States: N. p., 2015.
Web. doi:10.1021/jp511080q.
Li, Jun, Sham, Tsun-Kong, Ye, Yifan, Zhu, Junfa, & Guo, Jinghua. Structural and Optical Interplay of Palladium-Modified TiO 2 Nanoheterostructure. United States. https://doi.org/10.1021/jp511080q
Li, Jun, Sham, Tsun-Kong, Ye, Yifan, Zhu, Junfa, and Guo, Jinghua. Mon .
"Structural and Optical Interplay of Palladium-Modified TiO 2 Nanoheterostructure". United States. https://doi.org/10.1021/jp511080q. https://www.osti.gov/servlets/purl/1512161.
@article{osti_1512161,
title = {Structural and Optical Interplay of Palladium-Modified TiO 2 Nanoheterostructure},
author = {Li, Jun and Sham, Tsun-Kong and Ye, Yifan and Zhu, Junfa and Guo, Jinghua},
abstractNote = {The electronic structure and optical properties of Pd-modified TiO2 nanotubes (NTs) with a vertically aligned nanotubular structure grown by a two-step electrochemical anodization method have been studied using X-ray spectroscopy. X-ray absorption near-edge structure (XANES) at the Ti L3,2- and O K-edges was used to investigate the TiO2 NTs before and after Pd modification. It was found that Pd nanoparticles (NPs) are uniformly coated on the NT surface. The Pd L3-edge of the deposited Pd NPs shows a more intense whiteline and a blue shift for the Pd L3-edge absorption threshold relative to Pd metal, indicating charge depletion from the Pd 4d orbital as a result NP formation. The lattice of Pd is slightly contracted upon NP formation, although it remains fcc as revealed by extended X-ray absorption fine structure (EXAFS) analysis at the Pd K-edge. X-ray-excited optical luminescence (XEOL) together with XANES with element and site specificity was used to study the optical luminescence from TiO2 NTs. It was found that the defect-originated XEOL intensity dropped noticeably in the Pd NP-coated NTs, suggesting a Pd NP–TiO2-interaction-mediated reduction in the radiative recombination of electrons and holes. Finally, further evidence is provided by Ti 2p resonant inelastic X-ray scattering (RIXS), in which no low-energy loss features (d–d transitions) were observed. The implications of these results are discussed.},
doi = {10.1021/jp511080q},
journal = {Journal of Physical Chemistry. C},
number = 4,
volume = 119,
place = {United States},
year = {Mon Jan 05 00:00:00 EST 2015},
month = {Mon Jan 05 00:00:00 EST 2015}
}
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Figures / Tables:
Figure 1: (a) Ti L3,2-edge and (b) O K-edge XANES spectra of APNT, NT450, PCNT450, commercial anatase and rutile (Sigma-Aldrich); All spectra are normalized to the edge jump (flat region of the absorption above the threshold); All except the APNT are shifted vertically for clarity.
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