Anomalous Self-Assembly and Ion Transport in Nanostructured Organic–Inorganic Solid Electrolytes

Sethi, Gurmukh K.; Jiang, Xi; Chakraborty, Rohan; Loo, Whitney S.; Villaluenga, Irune; Balsara, Nitash P.

doi:10.1021/acsmacrolett.8b00583

Title: Anomalous Self-Assembly and Ion Transport in Nanostructured Organic–Inorganic Solid Electrolytes

Journal Article · Tue Aug 14 00:00:00 EDT 2018 · ACS Macro Letters

DOI:https://doi.org/10.1021/acsmacrolett.8b00583· OSTI ID:1464098

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Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Energy Storage Research (JCESR) and Materials Sciences Division
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Energy Storage Research (JCESR), Materials Sciences Division and Energy Storage and Distributed Resources Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering

Nanostructured solid electrolytes containing ion-conducting domains and rigid nonconducting domains are obtained by block copolymer self-assembly. Here, we report on the synthesis and characteristics of mixtures of a hybrid diblock copolymer with an organic and inorganic block: poly(ethylene oxide)-b-poly(acryloisobutyl polyhedral oligomeric silsesquioxane) (PEO-POSS) and a lithium salt. In the neat state, PEO-POSS exhibits a classical order-to-disorder transition upon heating. Dilute electrolytes exhibit a dramatic reversal; a disorder-to-order transition upon heating is obtained, indicating that the addition of salt fundamentally changes interactions between the organic and inorganic chains. At higher salt concentrations, the electrolytes primarily form a lamellar phase. Coexisting lamellae and cylinders are found at intermediate salt concentrations and high temperatures. The conductivity and shear modulus of PEO-POSS are significantly higher than that of an all-organic block copolymer electrolyte with similar molecular weight and morphology, demonstrating that organic-inorganic block copolymers provide a promising route for developing the next generation of solid electrolytes for lithium batteries.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515

OSTI ID:: 1464098

Alternate ID(s):: OSTI ID: 1601191

Journal Information:: ACS Macro Letters, Vol. 7, Issue 9; ISSN 2161-1653

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 21 works

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Ion diffusion across a disorder-to-order phase transition in a poly(ethylene oxide)- b -poly(silsesquioxane) block copolymer electrolyte Timachova, Ksenia; Sethi, Gurmukh K.; Bhattacharya, Rajashree Molecular Systems Design & Engineering, Vol. 4, Issue 2 https://doi.org/10.1039/c8me00077h	journal	January 2019
Optimizing the monomer structure of polyhedral oligomeric silsesquioxane for ion transport in hybrid organic–inorganic block copolymers Gao, Kevin W.; Jiang, Xi; Hoffman, Zach J. Journal of Polymer Science, Vol. 58, Issue 2 https://doi.org/10.1002/pol.20190073	journal	January 2020
Superlattice by charged block copolymer self-assembly Shim, Jimin; Bates, Frank S.; Lodge, Timothy P. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-10141-z	journal	May 2019

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Title: Anomalous Self-Assembly and Ion Transport in Nanostructured Organic–Inorganic Solid Electrolytes

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