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DOE OSTI · 3374393

Reversible self-assembly of small molecules for recyclable solid-state battery electrolytes

Cho, Yukio [Stanford University, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Massachusetts Institute of Technology, Cambridge, MA (United States)] (ORCID:000000030919692X)·Fincher, Cole D. [Massachusetts Institute of Technology, Cambridge, MA (United States)]·Lamour, Guillaume [Université Paris-Saclay, Evry-Courcouronnes (France)] (ORCID:0000000293315532)·Christoff-Tempesta, Ty [University of California, Irvine, CA (United States); Massachusetts Institute of Technology, Cambridge, MA (United States)] (ORCID:0000000265516599)·Zuo, Xiaobing [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000201344804)·Chiang, Yet-Ming [Massachusetts Institute of Technology, Cambridge, MA (United States)] (ORCID:0000000208337674)·Ortony, Julia H. [University of California San Diego, La Jolla, CA (United States); Massachusetts Institute of Technology, Cambridge, MA (United States)] (ORCID:0000000174466207)
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Abstract

Performance often overshadows recyclability in contemporary battery designs, leading to sustainability challenges. Preemptive strategies integrating recyclable chemistry from the outset are thus increasingly critical for addressing the complexities in conventional recycling. Here we harness bio-inspired molecular self-assembly to create inherently recyclable battery materials. We use aramid amphiphiles that self-assemble in water through strong, collective hydrogen bonding and π–π stacking, forming air-stable, high-aspect-ratio nanoribbons with gigapascal-level stiffness. When processed into bulk solid-state electrolytes, these nanoribbons retain their ordered molecular arrangement and exhibit total conductivities of 1.6 × 10 −4 S cm −1 at 50 °C, Young’s moduli of 70 MPa and toughness values of 1 MJ m −3 , despite being stabilized solely by reversible non-covalent bonds. We further demonstrate clean separation of battery components by exposing used cells to an organic solvent, which disrupts the non-covalent cohesion and reverts all battery components to their original forms. Furthermore, this study underscores the potential of molecular self-assembly for specialized recyclable designs in energy storage applications.

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Cho, Yukio [Stanford University, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Massachusetts Institute of Technology, Cambridge, MA (United States)] (ORCID:000000030919692X), Fincher, Cole D. [Massachusetts Institute of Technology, Cambridge, MA (United States)], Lamour, Guillaume [Université Paris-Saclay, Evry-Courcouronnes (France)] (ORCID:0000000293315532), Christoff-Tempesta, Ty [University of California, Irvine, CA (United States); Massachusetts Institute of Technology, Cambridge, MA (United States)] (ORCID:0000000265516599), Zuo, Xiaobing [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000201344804), Chiang, Yet-Ming [Massachusetts Institute of Technology, Cambridge, MA (United States)] (ORCID:0000000208337674), Ortony, Julia H. [University of California San Diego, La Jolla, CA (United States); Massachusetts Institute of Technology, Cambridge, MA (United States)] (ORCID:0000000174466207). 2025-08-28. Reversible self-assembly of small molecules for recyclable solid-state battery electrolytes. https://doi.org/10.1038/s41557-025-01917-6

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