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Title: Understanding the Effect of Preparative Approaches in the Formation of “Flower-like” Li 4Ti 5O 12 —Multiwalled Carbon Nanotube Composite Motifs with Performance as High-Rate Anode Materials for Li-Ion Battery Applications

Herein we highlight the significance of nanoscale attachment modality as an important determinant of observed electrochemical performance. Specifically, controlled loading ratios of multi-walled carbon nanotubes (MWNTs) have been successfully anchored onto the surfaces of a unique “flower-like” Li 4Ti 5O 12 (LTO) micro-scale sphere motif, for the first time, using a number of different and distinctive preparative approaches, including (i) a sonication method, (ii) an in situ direct-deposition approach, (iii) a covalent attachment protocol, as well as (iv) a π-π interaction strategy. In terms of structural characterization, the composites generated by physical sonication as well as non-covalent π-π interactions retained the intrinsic hierarchical “flower-like” morphology and exhibited a similar crystallinity profile as compared with that of pure LTO. By comparison, the composite prepared by an in situ direct deposition approach yielded not only a fragmented LTO structure, likely due to the possible interfering presence of the MWNTs themselves during the relevant hydrothermal reaction, but also a larger crystallite size, owing to the higher annealing temperature associated with its preparation. Finally, the composite created via covalent attachment was covered with an amorphous insulating linker, which probably led to a decreased contact area between the LTO and the MWNTs and hence, amore » lower crystallinity in the resulting composite. In addition electrode tests suggested that the composite generated by π-π interactions out-performed the other three analogous heterostructures, due to a smaller charge transfer resistance as well as a faster Li-ion diffusion. In particular, the LTO-MWNT composite, produced by π-π interactions, exhibited a reproducibly high rate capability as well as a reliably solid cycling stability, delivering 132 mA h g -1 at 50 C, after 100 discharge/charge cycles, including 40 cycles at a high (>20 C) rate. To conclude, such data denote the highest electrochemical performance measured to date as compared with any LTO-carbon nanotube-based composite materials previously reported, under high discharge rate conditions, and tangibly underscore the correlation between preparative methodology and the resulting performance metrics.« less
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [2] ;  [3] ;  [4]
  1. State University of New York at Stony Brook, Stony Brook, NY (United States). Department of Chemistry
  2. State University of New York at Stony Brook, Stony Brook, NY (United States). Department of Chemistry and Department of Materials Science and Engineering
  3. State University of New York at Stony Brook, Stony Brook, NY (United States). Department of Chemistry and Department of Materials Science and Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Energy Sciences Directorate, Interdisciplinary Sciences Building
  4. State University of New York at Stony Brook, Stony Brook, NY (United States). Department of Chemistry ; Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Division
Publication Date:
Report Number(s):
BNL-114102-2017-JA
Journal ID: ISSN 0013-4651
Grant/Contract Number:
SC0012704; SC0012673
Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 2; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE
OSTI Identifier:
1376152

Wang, Lei, Zhang, Yiman, McBean, Coray L., Scofield, Megan E., Yin, Jiefu, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., and Wong, Stanislaus S.. Understanding the Effect of Preparative Approaches in the Formation of “Flower-like” Li4Ti5O12 —Multiwalled Carbon Nanotube Composite Motifs with Performance as High-Rate Anode Materials for Li-Ion Battery Applications. United States: N. p., Web. doi:10.1149/2.1441702jes.
Wang, Lei, Zhang, Yiman, McBean, Coray L., Scofield, Megan E., Yin, Jiefu, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., & Wong, Stanislaus S.. Understanding the Effect of Preparative Approaches in the Formation of “Flower-like” Li4Ti5O12 —Multiwalled Carbon Nanotube Composite Motifs with Performance as High-Rate Anode Materials for Li-Ion Battery Applications. United States. doi:10.1149/2.1441702jes.
Wang, Lei, Zhang, Yiman, McBean, Coray L., Scofield, Megan E., Yin, Jiefu, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., and Wong, Stanislaus S.. 2017. "Understanding the Effect of Preparative Approaches in the Formation of “Flower-like” Li4Ti5O12 —Multiwalled Carbon Nanotube Composite Motifs with Performance as High-Rate Anode Materials for Li-Ion Battery Applications". United States. doi:10.1149/2.1441702jes. https://www.osti.gov/servlets/purl/1376152.
@article{osti_1376152,
title = {Understanding the Effect of Preparative Approaches in the Formation of “Flower-like” Li4Ti5O12 —Multiwalled Carbon Nanotube Composite Motifs with Performance as High-Rate Anode Materials for Li-Ion Battery Applications},
author = {Wang, Lei and Zhang, Yiman and McBean, Coray L. and Scofield, Megan E. and Yin, Jiefu and Marschilok, Amy C. and Takeuchi, Kenneth J. and Takeuchi, Esther S. and Wong, Stanislaus S.},
abstractNote = {Herein we highlight the significance of nanoscale attachment modality as an important determinant of observed electrochemical performance. Specifically, controlled loading ratios of multi-walled carbon nanotubes (MWNTs) have been successfully anchored onto the surfaces of a unique “flower-like” Li4Ti5O12 (LTO) micro-scale sphere motif, for the first time, using a number of different and distinctive preparative approaches, including (i) a sonication method, (ii) an in situ direct-deposition approach, (iii) a covalent attachment protocol, as well as (iv) a π-π interaction strategy. In terms of structural characterization, the composites generated by physical sonication as well as non-covalent π-π interactions retained the intrinsic hierarchical “flower-like” morphology and exhibited a similar crystallinity profile as compared with that of pure LTO. By comparison, the composite prepared by an in situ direct deposition approach yielded not only a fragmented LTO structure, likely due to the possible interfering presence of the MWNTs themselves during the relevant hydrothermal reaction, but also a larger crystallite size, owing to the higher annealing temperature associated with its preparation. Finally, the composite created via covalent attachment was covered with an amorphous insulating linker, which probably led to a decreased contact area between the LTO and the MWNTs and hence, a lower crystallinity in the resulting composite. In addition electrode tests suggested that the composite generated by π-π interactions out-performed the other three analogous heterostructures, due to a smaller charge transfer resistance as well as a faster Li-ion diffusion. In particular, the LTO-MWNT composite, produced by π-π interactions, exhibited a reproducibly high rate capability as well as a reliably solid cycling stability, delivering 132 mA h g-1 at 50 C, after 100 discharge/charge cycles, including 40 cycles at a high (>20 C) rate. To conclude, such data denote the highest electrochemical performance measured to date as compared with any LTO-carbon nanotube-based composite materials previously reported, under high discharge rate conditions, and tangibly underscore the correlation between preparative methodology and the resulting performance metrics.},
doi = {10.1149/2.1441702jes},
journal = {Journal of the Electrochemical Society},
number = 2,
volume = 164,
place = {United States},
year = {2017},
month = {1}
}