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However, the intrinsic chemical incompatibility between the halide Li3InCl6 (LIC) and the sulfide Li6PS5Cl (LPSC) drives persistent In-centric interfacial reconstruction, leading to continuous impedance growth and electrochemical decay. Across an investigated Li3In1\u2013xYxCl6 series (nominal x = 0.05\u20130.20), we show that the nominal x = 0.10 composition generates an outward charge-enriched boundary on the outer Cl\u2013 sublattice, markedly improving interfacial compatibility. This localized electronic feature smooths the electrostatic landscape for Li+ migration, increases the room-temperature ionic conductivity to 1.5 mS cm\u20131, and effectively suppresses the sustained inward propagation of sulfide-associated interfacial reconstruction. As a result, the corresponding halide\/sulfide interface develops a much shallower and more spatially confined reconstruction layer. All-solid-state cells based on the optimized chloride electrolyte deliver a specific capacity of 175 mAh g\u20131 at 1C, with about 88.2% capacity retention after 1000 cycles. These findings establish outward charge-boundary engineering as a route to simultaneously improve bulk ion transport and suppress interfacial degradation in reactive halide\u2013sulfide solid electrolytes.<\/jats:p>","DOI":"10.1021\/acs.inorgchem.6c03434","type":"journal-article","created":{"date-parts":[[2026,9,14]],"date-time":"2026-09-14T16:01:45Z","timestamp":1789401705000},"page":"22631-22643","source":"Crossref","is-referenced-by-count":0,"title":["Outward Charge-Enriched\nBoundaries Stabilize Halide\u2013Sulfide\nSolid\u2013Electrolyte Interfaces"],"prefix":"10.1021","volume":"65","author":[{"given":"Qingkun","family":"Zhu","sequence":"first","affiliation":[{"name":"Central South University , , ,","place":["Changsha, P. R. China, 410083"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenrui","family":"Hu","sequence":"additional","affiliation":[{"name":"Central South University , , ,","place":["Changsha, P. R. China, 410083"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7522-4728","authenticated-orcid":true,"given":"Fenghua","family":"Zheng","sequence":"additional","affiliation":[{"name":"Guangxi Normal University , , ,","place":["Guilin, P. R. China, 541004"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyou","family":"He","sequence":"additional","affiliation":[{"name":"Central South University , , ,","place":["Changsha, P. R. China, 410083"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiming","family":"Xiao","sequence":"additional","affiliation":[{"name":"Central South University , , ,","place":["Changsha, P. R. 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China, 410083"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3516-3817","authenticated-orcid":true,"given":"Xinghui","family":"Liang","sequence":"additional","affiliation":[{"name":"Central South University , , ,","place":["Changsha, P. R. China, 410083"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Baishan","family":"Chen","sequence":"additional","affiliation":[{"name":"Central South University , , ,","place":["Changsha, P. R. China, 410083"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3542-0243","authenticated-orcid":true,"given":"Changsheng","family":"An","sequence":"additional","affiliation":[{"name":"Changsha University , , ,","place":["Changsha, P. R. China, 410022"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiaqi","family":"Wang","sequence":"additional","affiliation":[{"name":"Nankai University , , ,","place":["Tianjin, P. R. 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