A chemical switch enabled autonomous two-stage crosslinking polymeric binder for high performance silicon anodes
Abstract
Silicon (Si) is a promising high-capacity anode material for high-energy-density lithium-ion batteries. However, the drastic volumetric changes of Si upon lithiation/delithiation hinder the practical use of Si anodes. Although adhesive polymeric binders, such as poly(acrylic acid) (PAA), mitigate this issue, the cycling performance of the fabricated Si anodes is still far from meeting the criteria of practical applications. In this study, we present a novel polymeric binder system for Si anodes consisting of PAA, a chemical switch (ammonia, NH3), and a crosslinker (branched polyethylenimine, PEI). The crosslinking between PAA and PEI is switched off in the slurry, which can then be turned on during electrode drying. Interestingly, the crosslinking reaction consists of two stages: ionic cross-linking (PAA-PEI-i) and covalent crosslinking (PAA-PEI-c) at a higher temperature (e.g., 130 °C). In half-cells, Si anodes fabricated using the PAA-PEI-c binder show a 67% increase in capacity retention compared to PAA anodes over 150 cycles at C/3 rate. The PAA-PEI-c binder also outperforms PAA in full cells. In addition, the chemical switch controlled crosslinking binder system also facilitates the slurry making process by avoiding early crosslinking. This system requires no additional steps compared to the conventional electrode lamination process, showing enormous potential for directmore »
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE
- OSTI Identifier:
- 1869939
- Alternate Identifier(s):
- OSTI ID: 1837091
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Materials Chemistry. A
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 3; Journal ID: ISSN 2050-7488
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; in situ crosslinking; lithium-ion battery; polymeric binder; silicon anode
Citation Formats
Shi, Zhangxing, Liu, Qian, Yang, Zhenzhen, Robertson, Lily A., Bheemireddy, Sambasiva R., Zhao, Yuyue, Zhang, Zhengcheng, and Zhang, Lu. A chemical switch enabled autonomous two-stage crosslinking polymeric binder for high performance silicon anodes. United States: N. p., 2021.
Web. doi:10.1039/d1ta07112b.
Shi, Zhangxing, Liu, Qian, Yang, Zhenzhen, Robertson, Lily A., Bheemireddy, Sambasiva R., Zhao, Yuyue, Zhang, Zhengcheng, & Zhang, Lu. A chemical switch enabled autonomous two-stage crosslinking polymeric binder for high performance silicon anodes. United States. https://doi.org/10.1039/d1ta07112b
Shi, Zhangxing, Liu, Qian, Yang, Zhenzhen, Robertson, Lily A., Bheemireddy, Sambasiva R., Zhao, Yuyue, Zhang, Zhengcheng, and Zhang, Lu. Mon .
"A chemical switch enabled autonomous two-stage crosslinking polymeric binder for high performance silicon anodes". United States. https://doi.org/10.1039/d1ta07112b. https://www.osti.gov/servlets/purl/1869939.
@article{osti_1869939,
title = {A chemical switch enabled autonomous two-stage crosslinking polymeric binder for high performance silicon anodes},
author = {Shi, Zhangxing and Liu, Qian and Yang, Zhenzhen and Robertson, Lily A. and Bheemireddy, Sambasiva R. and Zhao, Yuyue and Zhang, Zhengcheng and Zhang, Lu},
abstractNote = {Silicon (Si) is a promising high-capacity anode material for high-energy-density lithium-ion batteries. However, the drastic volumetric changes of Si upon lithiation/delithiation hinder the practical use of Si anodes. Although adhesive polymeric binders, such as poly(acrylic acid) (PAA), mitigate this issue, the cycling performance of the fabricated Si anodes is still far from meeting the criteria of practical applications. In this study, we present a novel polymeric binder system for Si anodes consisting of PAA, a chemical switch (ammonia, NH3), and a crosslinker (branched polyethylenimine, PEI). The crosslinking between PAA and PEI is switched off in the slurry, which can then be turned on during electrode drying. Interestingly, the crosslinking reaction consists of two stages: ionic cross-linking (PAA-PEI-i) and covalent crosslinking (PAA-PEI-c) at a higher temperature (e.g., 130 °C). In half-cells, Si anodes fabricated using the PAA-PEI-c binder show a 67% increase in capacity retention compared to PAA anodes over 150 cycles at C/3 rate. The PAA-PEI-c binder also outperforms PAA in full cells. In addition, the chemical switch controlled crosslinking binder system also facilitates the slurry making process by avoiding early crosslinking. This system requires no additional steps compared to the conventional electrode lamination process, showing enormous potential for direct adoption in large-scale manufacturing.},
doi = {10.1039/d1ta07112b},
journal = {Journal of Materials Chemistry. A},
number = 3,
volume = 10,
place = {United States},
year = {Mon Dec 06 00:00:00 EST 2021},
month = {Mon Dec 06 00:00:00 EST 2021}
}
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