Green Electrode Processing Enabled by Fluoro-Free Multifunctional Binders for Lithium-Ion Batteries

Jin, Xiuyu [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000178452371); Zhu, Ziting [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]; Miao, Qiusu [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]; Fang, Chen [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]; Huang, Di [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]; Giovine, Raynald [University of California, Berkeley, CA (United States)]; Chen, Linfeng [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry]; Dun, Chaochao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry]; Urban, Jeffrey J. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry]; Fu, Yanbao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]; Li, Defu [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]; Liu, Katie [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]; Wang, Yunfei [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Univ. of Southern Mississippi, Hattiesburg, MS (United States)]; Zhu, Tianyu [Clemson Univ., SC (United States)]; Zhu, Chenhui [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)]; Tong, Wei [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]; Liu, Gao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000168860507)

doi:10.1002/advs.202416995

DOE OSTI · 2557481

Green Electrode Processing Enabled by Fluoro-Free Multifunctional Binders for Lithium-Ion Batteries

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Abstract

The eco-friendly processing of conjugated polymer binder for lithium-ion batteries demands improved polymer solubility by introducing functional moieties, while this strategy will concurrently sacrifice polymer conductivity. Employing the polyfluorene-based binder poly(2,7-9,9 (di(oxy-2,5,8-trioxadecane))fluorene) (PFO), soluble in water-ethanol mixtures, a novel approach is presented to solve this trade-off, which features integration of aqueous solution processing with subsequent controlled thermal-induced cleavage of solubilizing side chains, to produce hierarchically ordered structures (HOS). The thermal processing can enhance the intermolecular π–π stacking of polyfluorene backbone for better electrochemical performance. Notably, HOS-PFO demonstrated a substantial 6–7 orders of magnitude enhancement in electronic conductivity, showcasing its potential as a functional binder for lithium-ion batteries. As an illustration, HOS-PFO protected SiOx anodes, utilizing in situ side chain decomposition of PFO surrounding SiOx particles after aqueous processing are fabricated. HOS-PFO contributed to the stable cycling and high-capacity retention of practical SiOx anodes (3.0 mAh cm -2 ), without the use of any conducting carbon additives or fluorinated electrolyte additives. It is proposed that this technique represents a universal approach for fabricating electrodes with conjugated polymer binders from aqueous solutions without compromising conductivity.

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25 ENERGY STORAGE conductive binder conjugated polymer green processing hierarchically ordered structure lithium-ion battery

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Jin, Xiuyu [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000178452371), Zhu, Ziting [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Miao, Qiusu [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Fang, Chen [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Huang, Di [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Giovine, Raynald [University of California, Berkeley, CA (United States)], Chen, Linfeng [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry], Dun, Chaochao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry], Urban, Jeffrey J. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry], Fu, Yanbao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Li, Defu [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Liu, Katie [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Wang, Yunfei [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Univ. of Southern Mississippi, Hattiesburg, MS (United States)], Zhu, Tianyu [Clemson Univ., SC (United States)], Zhu, Chenhui [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)], Tong, Wei [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Liu, Gao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000168860507). 2025-03-06. Green Electrode Processing Enabled by Fluoro-Free Multifunctional Binders for Lithium-Ion Batteries. https://doi.org/10.1002/advs.202416995

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