Restorable Neutralization of Poly(acrylic acid) Binders toward Balanced Processing Properties and Cycling Performance for Silicon Anodes in Lithium-Ion BatteriesClick to copy article linkArticle link copied!
- Zhangxing ShiZhangxing ShiChemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United StatesMore by Zhangxing Shi
- Sisi JiangSisi JiangChemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United StatesMore by Sisi Jiang
- Lily A. RobertsonLily A. RobertsonChemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United StatesJoint Center for Energy Storage Research, 9700 South Cass Avenue, Lemont, Illinois 60439, United StatesMore by Lily A. Robertson
- Yuyue ZhaoYuyue ZhaoChemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United StatesJoint Center for Energy Storage Research, 9700 South Cass Avenue, Lemont, Illinois 60439, United StatesMore by Yuyue Zhao
- Erik SarnelloErik SarnelloDepartment of Chemistry and Biochemistry, Northern Illinois University, DeKalb, Illinois 60115, United StatesMore by Erik Sarnello
- Tao LiTao LiDepartment of Chemistry and Biochemistry, Northern Illinois University, DeKalb, Illinois 60115, United StatesX-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Tao Li
- Wei ChenWei ChenInstitute for Molecular Engineering and Materials Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United StatesInstitute for Molecular Engineering, The University of Chicago, 5640 South Ellis Avenue, Chicago, Illinois 60637, United StatesMore by Wei Chen
- Zhengcheng ZhangZhengcheng ZhangChemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United StatesJoint Center for Energy Storage Research, 9700 South Cass Avenue, Lemont, Illinois 60439, United StatesMore by Zhengcheng Zhang
- Lu Zhang*Lu Zhang*Email: [email protected]Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United StatesJoint Center for Energy Storage Research, 9700 South Cass Avenue, Lemont, Illinois 60439, United StatesMore by Lu Zhang
Abstract

Neutralization of poly(acrylic acid) (PAA)-based binders using lithium hydroxide is a common strategy for fabricating silicon anode laminates, which improves rheological properties of slurries toward high-quality electrode laminates. However, the significantly increased basicity causes degradation of Si particles while the irreversible conversion of carboxylic acid groups to lithium carboxylates undermines the binding strength, collectively leading to adverse cycling performance of the fabricated Si anodes. Herein, a novel neutralization process for PAA binders is developed. A weak base, ammonia (NH3), was discovered as a neutralizing agent that still promotes rheological response of binder solutions but results in a reduced pH increase. Interestingly, the resulting ammonium carboxylate groups may cleave during the drying process to restore the neutralized PAA (PAA-NH3) binders to their pristine states. The best-performing composition of 50% neutralization (PAA-50%NH3) provides comparable rheological response as a PAA-Li binder as well as much improved cycling performance. The half-cells using the PAA-50%NH3 binder can deliver 60% capacity retention over 100 cycles at C/3 rate, affording a 23.8% increase compared to PAA-Li half-cells. This restorable neutralization process of PAA binders represents an innovative strategy of mitigating issues from slurry processing of Si particles to achieve concurrent improvements in high-quality lamination and cycling performance.
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