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However, the interphase in all\u2010solid\u2010state batteries (ASSBs) arises from mutual electrochemical decomposition between the anode and solid electrolyte, yielding unpredictable composition, poor ionic conductivity, and insufficient mechanical compliance. Instead of suppressing this interfacial reaction, we introduce a reactive anolyte design strategy in which vacancy\u2010rich \u03b2\u2010Li\n                    <jats:sub>3<\/jats:sub>\n                    N undergoes a controlled in situ interfacial reaction with Si, resulting in a purpose\u2010built lithium nitridosilicate interlayer directly on the surfaces of Si particles within the composite anode. This interlayer with the anolyte simultaneously establishes fast Li\n                    <jats:sup>+<\/jats:sup>\n                    transport pathways, suppresses electrochemical sintering, and accommodates large volumetric strain. A pre\u2010lithiation protocol further shifts the anode operation window into the kinetically favorable region and supplements the Li inventory. The resulting composite Si anode paired with a LiCoO\n                    <jats:sub>2<\/jats:sub>\n                    cathode delivers outstanding rate capability (19C, current density of 25.5 mA\/cm\n                    <jats:sup>2<\/jats:sup>\n                    ), long cycling stability (over 5000 cycles), and high areal capacity (above 10 mAh\/cm\n                    <jats:sup>2<\/jats:sup>\n                    ). Beyond the Li\u2010Si\u2010N system, the reactive anolyte principle could be extended to other alloy\u2010 and conversion\u2010type active materials, offering both a practical solution to the Si anode interface problem and a conceptual framework for rational interphase engineering in next\u2010generation ASSBs.\n                  <\/jats:p>","DOI":"10.1002\/adma.75015","type":"journal-article","created":{"date-parts":[[2026,9,16]],"date-time":"2026-09-16T06:45:13Z","timestamp":1789541113000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["In Situ Lithium Nitridosilicate Interlayer via Reactive Anolyte Design for All\u2010Solid\u2010State Silicon Anodes"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-2106-6861","authenticated-orcid":false,"given":"Tongtai","family":"Ji","sequence":"first","affiliation":[{"name":"Department of Mechanical and Industrial Engineering Northeastern University  Boston Massachusetts USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huanyao","family":"Ge","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Chemical Biology Northeastern University  Boston Massachusetts USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Luisa","family":"Gomes","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Chemical Biology Northeastern University  Boston Massachusetts USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6808-1941","authenticated-orcid":false,"given":"Conan","family":"Weiland","sequence":"additional","affiliation":[{"name":"Material Measurement Laboratory National Institute of Standards and Technology  Gaithersburg Maryland USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5511-2083","authenticated-orcid":false,"given":"Aswin kumar","family":"Anbalagan","sequence":"additional","affiliation":[{"name":"National Synchrotron Light Source II Brookhaven National Laboratory  Upton New York USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9001-5991","authenticated-orcid":false,"given":"Jochem","family":"Struppe","sequence":"additional","affiliation":[{"name":"Bruker BioSpin Corp.  Billerica Massachusetts USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jason","family":"Guo","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Chemical Biology Northeastern University  Boston Massachusetts USA"},{"name":"Barnett Institute for Chemical and Biological Analysis Northeastern University  Boston Massachusetts USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Andrew L.","family":"Walter","sequence":"additional","affiliation":[{"name":"National Synchrotron Light Source II Brookhaven National Laboratory  Upton New York USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2980-7655","authenticated-orcid":false,"given":"Sanjeev","family":"Mukerjee","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Chemical Biology Northeastern University  Boston Massachusetts 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