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Title: Low-Tortuosity Thick Electrodes with Active Materials Gradient Design for Enhanced Energy Storage

Abstract

The ever-growing energy demand of modern society calls for the development of high-loading and high-energy-density batteries, and substantial research efforts are required to optimize electrode microstructures for improved energy storage. Low-tortuosity architecture proves effective in promoting charge transport kinetics in thick electrodes; however, heterogeneous electrochemical mass transport along the depth direction is inevitable, especially at high C-rates. In this work, we create an active material gradient in low-tortuosity electrodes along ion-transport direction to compensate for uneven reaction kinetics and the nonuniform lithiation/delithiation process in thick electrodes. The gradual decrease of active material concentration from the separator to the current collector reduces the integrated ion diffusion distance and accelerates the electrochemical reaction kinetics, leading to improved rate capabilities. Further, the structure advantages combining low-tortuosity pores and active material gradient offer high mass loading (60 mg cm–2) and enhanced performance. Comprehensive understanding of the effect of active material gradient architecture on electrode kinetics has been elucidated by electrochemical characterization and simulations, which can be useful for development of batteries with high-energy/power densities.

Authors:
 [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [2];  [2];  [2];  [1]
+ Show Author Affiliations
  1. Univ. of Texas, Austin, TX (United States)
  2. Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties; Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1895071
Alternate Identifier(s):
OSTI ID: 1865650
Report Number(s):
BNL-223640-2022-JAAM
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
SC0012704; SC0012673; SC0021314
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 16; Journal Issue: 3; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; thick electrodes; gradient; low-turtuosity; reaction kinetics; ion diffusion; low-tortuosity

Citation Formats

Wu, Jingyi, Ju, Zhengyu, Zhang, Xiao, Xu, Xiao, Takeuchi, Kenneth J., Marschilok, Amy C., Takeuchi, Esther S., and Yu, Guihua. Low-Tortuosity Thick Electrodes with Active Materials Gradient Design for Enhanced Energy Storage. United States: N. p., 2022. Web. doi:10.1021/acsnano.2c00129.
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Wu, Jingyi, Ju, Zhengyu, Zhang, Xiao, Xu, Xiao, Takeuchi, Kenneth J., Marschilok, Amy C., Takeuchi, Esther S., & Yu, Guihua. Low-Tortuosity Thick Electrodes with Active Materials Gradient Design for Enhanced Energy Storage. United States. https://doi.org/10.1021/acsnano.2c00129
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Wu, Jingyi, Ju, Zhengyu, Zhang, Xiao, Xu, Xiao, Takeuchi, Kenneth J., Marschilok, Amy C., Takeuchi, Esther S., and Yu, Guihua. Wed . "Low-Tortuosity Thick Electrodes with Active Materials Gradient Design for Enhanced Energy Storage". United States. https://doi.org/10.1021/acsnano.2c00129. https://www.osti.gov/servlets/purl/1895071.
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@article{osti_1895071,
title = {Low-Tortuosity Thick Electrodes with Active Materials Gradient Design for Enhanced Energy Storage},
author = {Wu, Jingyi and Ju, Zhengyu and Zhang, Xiao and Xu, Xiao and Takeuchi, Kenneth J. and Marschilok, Amy C. and Takeuchi, Esther S. and Yu, Guihua},
abstractNote = {The ever-growing energy demand of modern society calls for the development of high-loading and high-energy-density batteries, and substantial research efforts are required to optimize electrode microstructures for improved energy storage. Low-tortuosity architecture proves effective in promoting charge transport kinetics in thick electrodes; however, heterogeneous electrochemical mass transport along the depth direction is inevitable, especially at high C-rates. In this work, we create an active material gradient in low-tortuosity electrodes along ion-transport direction to compensate for uneven reaction kinetics and the nonuniform lithiation/delithiation process in thick electrodes. The gradual decrease of active material concentration from the separator to the current collector reduces the integrated ion diffusion distance and accelerates the electrochemical reaction kinetics, leading to improved rate capabilities. Further, the structure advantages combining low-tortuosity pores and active material gradient offer high mass loading (60 mg cm–2) and enhanced performance. Comprehensive understanding of the effect of active material gradient architecture on electrode kinetics has been elucidated by electrochemical characterization and simulations, which can be useful for development of batteries with high-energy/power densities.},
doi = {10.1021/acsnano.2c00129},
journal = {ACS Nano},
number = 3,
volume = 16,
place = {United States},
year = {Wed Mar 02 00:00:00 EST 2022},
month = {Wed Mar 02 00:00:00 EST 2022}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acsnano.2c00129
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