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Title: Effects of proton irradiation on structural and electrochemical charge storage properties of TiO 2 nanotube electrodes for lithium-ion batteries

The effects of proton irradiation on nanostructured metal oxides have been investigated. Recent studies suggest that the presence of structural defects (e.g. vacancies and interstitials) in metal oxides may enhance the material's electrochemical charge storage capacity. A new approach to introduce defects in electrode materials is to use ion irradiation as it can produce a supersaturation of point defects in the target material. In this work we report the effect of low-energy proton irradiation on amorphous TiO 2 nanotube electrodes at both room temperature and high temperature (250 °C). Upon room temperature irradiation the nanotubes demonstrate an irradiation-induced phase transformation to a mixture of amorphous, anatase, and rutile domains while showing a 35% reduction in capacity compared to anatase TiO 2. On the other hand, the high temperature proton irradiation induced a disordered rutile phase within the nanotubes as characterized by Raman spectroscopy and transmission electron microscopy, which displays an improved capacity by 20% at ~240 mA h g –1 as well as improved rate capability compared to an unirradiated anatase sample. Voltammetric sweep data were used to determine the contributions from diffusion-limited intercalation and capacitive processes and it was found that the electrodes after irradiation had more contributions frommore » diffusion in lithium charge storage. Finally, our work suggests that tailoring the defect generation through ion irradiation within metal oxide electrodes could present a new avenue for designing advanced electrode materials.« less
Authors:
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Publication Date:
Report Number(s):
BNL-113759-2017-JA; LA-UR-18-21408
Journal ID: ISSN 2050-7488; JMCAET; R&D Project: 16060; 16060; KC0403020
Grant/Contract Number:
SC00112704; AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 2017; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC). Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
29 ENERGY PLANNING, POLICY, AND ECONOMY; TiO2; lithium ion battery; proton Irradiation; Center for Functional Nanomaterials; 25 ENERGY STORAGE; Material Science
OSTI Identifier:
1427393
Alternate Identifier(s):
OSTI ID: 1351743

Smith, Kassiopeia A., Savva, Andreas I., Deng, Changjian, Wharry, Janelle P., Hwang, Sooyeon, Su, Dong, Wang, Yongqiang, Gong, Jue, Xu, Tao, Butt, Darryl P., and Xiong, Hui. Effects of proton irradiation on structural and electrochemical charge storage properties of TiO 2 nanotube electrodes for lithium-ion batteries. United States: N. p., Web. doi:10.1039/C7TA01026E.
Smith, Kassiopeia A., Savva, Andreas I., Deng, Changjian, Wharry, Janelle P., Hwang, Sooyeon, Su, Dong, Wang, Yongqiang, Gong, Jue, Xu, Tao, Butt, Darryl P., & Xiong, Hui. Effects of proton irradiation on structural and electrochemical charge storage properties of TiO 2 nanotube electrodes for lithium-ion batteries. United States. doi:10.1039/C7TA01026E.
Smith, Kassiopeia A., Savva, Andreas I., Deng, Changjian, Wharry, Janelle P., Hwang, Sooyeon, Su, Dong, Wang, Yongqiang, Gong, Jue, Xu, Tao, Butt, Darryl P., and Xiong, Hui. 2017. "Effects of proton irradiation on structural and electrochemical charge storage properties of TiO 2 nanotube electrodes for lithium-ion batteries". United States. doi:10.1039/C7TA01026E. https://www.osti.gov/servlets/purl/1427393.
@article{osti_1427393,
title = {Effects of proton irradiation on structural and electrochemical charge storage properties of TiO 2 nanotube electrodes for lithium-ion batteries},
author = {Smith, Kassiopeia A. and Savva, Andreas I. and Deng, Changjian and Wharry, Janelle P. and Hwang, Sooyeon and Su, Dong and Wang, Yongqiang and Gong, Jue and Xu, Tao and Butt, Darryl P. and Xiong, Hui},
abstractNote = {The effects of proton irradiation on nanostructured metal oxides have been investigated. Recent studies suggest that the presence of structural defects (e.g. vacancies and interstitials) in metal oxides may enhance the material's electrochemical charge storage capacity. A new approach to introduce defects in electrode materials is to use ion irradiation as it can produce a supersaturation of point defects in the target material. In this work we report the effect of low-energy proton irradiation on amorphous TiO2 nanotube electrodes at both room temperature and high temperature (250 °C). Upon room temperature irradiation the nanotubes demonstrate an irradiation-induced phase transformation to a mixture of amorphous, anatase, and rutile domains while showing a 35% reduction in capacity compared to anatase TiO2. On the other hand, the high temperature proton irradiation induced a disordered rutile phase within the nanotubes as characterized by Raman spectroscopy and transmission electron microscopy, which displays an improved capacity by 20% at ~240 mA h g–1 as well as improved rate capability compared to an unirradiated anatase sample. Voltammetric sweep data were used to determine the contributions from diffusion-limited intercalation and capacitive processes and it was found that the electrodes after irradiation had more contributions from diffusion in lithium charge storage. Finally, our work suggests that tailoring the defect generation through ion irradiation within metal oxide electrodes could present a new avenue for designing advanced electrode materials.},
doi = {10.1039/C7TA01026E},
journal = {Journal of Materials Chemistry. A},
number = ,
volume = 2017,
place = {United States},
year = {2017},
month = {3}
}

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