A chemical switch enabled autonomous two-stage crosslinking polymeric binder for high performance silicon anodes

Shi, Zhangxing; Liu, Qian; Yang, Zhenzhen; Robertson, Lily A.; Bheemireddy, Sambasiva R.; Zhao, Yuyue; Zhang, Zhengcheng; Zhang, Lu

doi:10.1039/d1ta07112b

Title: A chemical switch enabled autonomous two-stage crosslinking polymeric binder for high performance silicon anodes

Journal Article · Mon Dec 06 00:00:00 EST 2021 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/d1ta07112b· OSTI ID:1869939

Shi, Zhangxing ^[1]; Liu, Qian ^[1]; Yang, Zhenzhen ^[1];

^[1];

^[1]

Argonne National Lab. (ANL), Lemont, IL (United States)

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1869939

Alternate ID(s):: OSTI ID: 1837091

Journal Information:: Journal of Materials Chemistry. A, Vol. 10, Issue 3; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Title: A chemical switch enabled autonomous two-stage crosslinking polymeric binder for high performance silicon anodes

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