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Among them, LaCl3-based SSEs feature a non-close-packed lattice that provides intrinsically wide one-dimensional transport channels; however, their practical application is often constrained by rigid crystalline transport pathways and grain boundary resistance. Inspired by dual-anion engineering, by substituting LiCl with Li2O in Li0.388Ta0.238La0.475Cl3, a series of LaCl3-based composite electrolytes, Li2xTa0.25La0.5Cl2.75Ox (0.15 \u2264 x \u2264 0.2, LTLCO), were synthesized. Atomic and local structure analysis reveals that, although elements are uniformly distributed at the macroscopic level, distinct local structural variations exist. Oxygen preferentially coordinates with Ta to form distorted octahedral Ta\u2013Cl\u2013O polyhedra, while the LaCl3 framework maintains structural integrity as a rigid backbone. The optimized Li0.35Ta0.25La0.5Cl2.75O0.175 SSE achieves a high ionic conductivity of 2.05 mS cm\u20131 at 30 \u00b0C and exhibits superior mechanical deformability, effectively mitigating interfacial failure in ASSLBs. ASSLBs assembled with LiNi0.83Co0.11Mn0.06O2 (NCM83) cathodes demonstrate exceptional rate performance and long-term cycling stability with 83.4% capacity retention after 300 cycles.<\/jats:p>","DOI":"10.1021\/acsnano.6c06291","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T13:19:54Z","timestamp":1785849594000},"page":"21965-21974","source":"Crossref","is-referenced-by-count":0,"title":["Oxygen-Mediated\nNanocrystalline\u2013Amorphous LaCl\n                    <b>3<\/b>\n                    -Based\nComposite Electrolytes for All-Solid-State\nLithium Batteries"],"prefix":"10.1021","volume":"20","author":[{"given":"Enhui","family":"Han","sequence":"first","affiliation":[{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"Su","sequence":"additional","affiliation":[{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dongxiao","family":"Wang","sequence":"additional","affiliation":[{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing","family":"Wang","sequence":"additional","affiliation":[{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaochen","family":"Zhang","sequence":"additional","affiliation":[{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Feihu","family":"Zou","sequence":"additional","affiliation":[{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-0875-5803","authenticated-orcid":true,"given":"Siqi","family":"Xu","sequence":"additional","affiliation":[{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5188-6241","authenticated-orcid":true,"given":"Tu","family":"Lan","sequence":"additional","affiliation":[{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huican","family":"Mao","sequence":"additional","affiliation":[{"name":"Jilin University , , ,","place":["Changchun, China, 130012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2800-6001","authenticated-orcid":true,"given":"Bingkun","family":"Guo","sequence":"additional","affiliation":[{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shigang","family":"Lu","sequence":"additional","affiliation":[{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hong","family":"Li","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3229-1175","authenticated-orcid":true,"given":"Yingchun","family":"Lyu","sequence":"additional","affiliation":[{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]},{"name":"Nankai University , , ,","place":["Tianjin, China, 300071"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,30]]},"reference":[{"key":"2026081111135068300_cit1","doi-asserted-by":"publisher","first-page":"603","DOI":"10.1038\/s41586-025-09358-4","article-title":"Addressing the Safety\nof Next-Generation Batteries","volume":"645","author":"Yang","year":"2025","journal-title":"Nature"},{"key":"2026081111135068300_cit2","doi-asserted-by":"publisher","first-page":"101953","DOI":"10.1016\/j.joule.2025.101953","article-title":"Unveiling the Thermite-Driven Lithium\nFire Ignition in Solid-State Batteries","volume":"9","author":"Bertrand","year":"2025","journal-title":"Joule"},{"key":"2026081111135068300_cit3","doi-asserted-by":"publisher","first-page":"3221","DOI":"10.1021\/acsenergylett.0c01977","article-title":"Promising\nAll-Solid-State Batteries for Future Electric Vehicles","volume":"5","author":"Sun","year":"2020","journal-title":"ACS Energy Lett."},{"issue":"1","key":"2026081111135068300_cit4","doi-asserted-by":"publisher","first-page":"3807","DOI":"10.1038\/s41467-023-39522-1","article-title":"A Cost-Effective,\nIonically Conductive and Compressible Oxychloride Solid-State Electrolyte\nfor Stable All-Solid-State Lithium-Based Batteries","volume":"14","author":"Hu","year":"2023","journal-title":"Nat. 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New Halide Superionic Conductors for All-Solid-State Batteries","volume":"425","author":"Park","year":"2021","journal-title":"Chem. Eng. J."},{"key":"2026081111135068300_cit23","doi-asserted-by":"publisher","first-page":"1481","DOI":"10.1039\/D5EB00064E","article-title":"Halide-Based\nSolid Electrolytes: Opportunities and Challenges in the Synergistic\nDevelopment of All-Solid-State Li\/Na Batteries","volume":"1","author":"Tang","year":"2025","journal-title":"EES Batteries"},{"key":"2026081111135068300_cit24","doi-asserted-by":"publisher","first-page":"16427","DOI":"10.1002\/anie.201909805","article-title":"Water-Mediated Synthesis\nof a Superionic Halide Solid\nElectrolyte","volume":"58","author":"Li","year":"2019","journal-title":"Angew. Chem., Int. 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