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Solvent-Free Melt-Processed Cathode Mitigates Li Anode Instability in Polymer-Based Solid-State Batteries

Chen, Xi Chelsea (ORCID:0000000311887658)·Musgrove, Amanda L. (ORCID:0009000220910389)·Preefer, Molleigh B. [Stanford Synchrotron Radiation Lightsource; SLAC National Accelerator Laboratory] (ORCID:0000000236998613)·Moy, Alexandra C. (ORCID:0000000244025432)·Owensby, Kyra D. [The Bredesen Center for Interdisciplinary Research and Graduate Education; The University of Tennessee Knoxville]·Long, Oliver·Zhang, Pu [Department of Materials Science and Engineering; Stanford University]·Demchuk, Zoriana·Ward, Thomas Zac (ORCID:0000000210279186)·Armstrong, Beth L. (ORCID:0000000171493576)·Verma, Ankit [Energy Conversion and Storage Systems Center; National Renewable Energy Laboratory] (ORCID:0000000276108574)·Usseglio-Viretta, Francois [Energy Conversion and Storage Systems Center; National Renewable Energy Laboratory]·Colclasure, Andrew M. [Energy Conversion and Storage Systems Center; National Renewable Energy Laboratory] (ORCID:0000000295745106)·Sahore, Ritu·Nelson Weker, Johanna [Stanford Synchrotron Radiation Lightsource; SLAC National Accelerator Laboratory] (ORCID:0000000168563203)·Veith, Gabriel M. (ORCID:0000000251864461)
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Abstract

Solvent-free manufacturing of battery components is a promising alternative to traditional slurry processing for reducing the cost and environmental impact. In this work, we used twin-screw melt extrusion to fabricate a polymer-based high voltage composite cathode. The melt-processed cathode is dense (near zero porosity) and thick (65 μm) and has high active material loading (80 wt %). The active particles are distributed uniformly throughout the melt-processed cathode, unlike the traditional slurry-cast cathode, which exhibits inhomogeneous particle distribution. In the melt-processed cathode, polymer and carbon form separate phases, whereas in the slurry-cast cathode they blend into a single phase. Due to these structural differences, the melt-processed cathode shows smooth charge–discharge profiles, while the slurry-cast cathode shows noisy charging and soft-shorting behavior. In conclusion, this work highlights that twin-screw extrusion as a scalable, solvent-free manufacturing method is advantageous in producing uniform cathodes, which mitigates anode instability.

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25 ENERGY STORAGECompositesElectrochemical cellsElectrodesPolymer particlesPolymersbatterieslithiummelt-processingsolid-statetwin-screw extrusion

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Chen, Xi Chelsea (ORCID:0000000311887658), Musgrove, Amanda L. (ORCID:0009000220910389), Preefer, Molleigh B. [Stanford Synchrotron Radiation Lightsource; SLAC National Accelerator Laboratory] (ORCID:0000000236998613), Moy, Alexandra C. (ORCID:0000000244025432), Owensby, Kyra D. [The Bredesen Center for Interdisciplinary Research and Graduate Education; The University of Tennessee Knoxville], Long, Oliver, Zhang, Pu [Department of Materials Science and Engineering; Stanford University], Demchuk, Zoriana, Ward, Thomas Zac (ORCID:0000000210279186), Armstrong, Beth L. (ORCID:0000000171493576), Verma, Ankit [Energy Conversion and Storage Systems Center; National Renewable Energy Laboratory] (ORCID:0000000276108574), Usseglio-Viretta, Francois [Energy Conversion and Storage Systems Center; National Renewable Energy Laboratory], Colclasure, Andrew M. [Energy Conversion and Storage Systems Center; National Renewable Energy Laboratory] (ORCID:0000000295745106), Sahore, Ritu, Nelson Weker, Johanna [Stanford Synchrotron Radiation Lightsource; SLAC National Accelerator Laboratory] (ORCID:0000000168563203), Veith, Gabriel M. (ORCID:0000000251864461). 2025-06-12. Solvent-Free Melt-Processed Cathode Mitigates Li Anode Instability in Polymer-Based Solid-State Batteries. https://doi.org/10.1021/acsenergylett.5c00790

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