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This study reports a hybrid\u2010sulfonamide electrolyte (HSE) that can survive the aggressive chemistry of high\u2010voltage NMC811 and programs a self\u2010limiting inorganic interphase on Si by leveraging the electron\u2010limited onset at the Si||electrolyte junction. At first lithiation, the semiconductor characteristic and native SiO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    create a space\u2010charge (depletion) region, so the anionic\u2010structure\u2010like sulfonamides bias first\u2010electron reduction, seeding lithium halide\/chalcogenide inorganics that are electronically insulating yet Li\n                    <jats:sup>+<\/jats:sup>\n                    \u2010permeable. The resulting thin, dense layer suppresses electron tunneling, dissolution, and resists crack\u2010induced stress concentration during Si expansion\u2014thereby self\u2010limiting further growth. Consequently, NMC811||SmG coin cells with the HSE retain 80% capacity after 500 cycles at 4.5\u00a0V and \u22485 mAh cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and operate over a wide range of temperature from \u221240 to 60 \u00b0C, markedly outperforming the carbonate electrolyte. 1.4 Ah pouch cells maintain 80.0% of initial capacity after 1150 cycles and exhibit thermal stability up to 300 \u00b0C. This work establishes self\u2010limiting interphase formation on Si as a practical electrolyte design target for high\u2010energy LIBs.\n                  <\/jats:p>","DOI":"10.1002\/adma.202515562","type":"journal-article","created":{"date-parts":[[2025,11,17]],"date-time":"2025-11-17T08:38:34Z","timestamp":1763368714000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":25,"title":["4.5\u2010V\u2010Class Safe Lithium\u2010Ion Batteries with Silicon\u2010Majority\u2010Graphite Anodes Enabled by Self\u2010Limiting Interphase"],"prefix":"10.1002","volume":"38","author":[{"given":"Longji","family":"Xu","sequence":"first","affiliation":[{"name":"Center for Advancing Materials Performance from the Nanoscale (CAMP\u2010Nano) State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University  Xi'an Shaanxi 710049 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,11,17]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-46186-y"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-021-00792-y"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202402625"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.nxener.2024.100176"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-22662-7"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jechem.2024.12.048"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/nenergy.2016.113"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-024-01519-5"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-025-01734-8"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41557-024-01585-y"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202409431"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-023-01333-5"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-020-1972-y"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-019-1481-z"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-022-01055-0"},{"key":"e_1_2_7_16_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-023-01792-x"},{"key":"e_1_2_7_17_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-020-0601-1"},{"key":"e_1_2_7_18_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202310297"},{"key":"e_1_2_7_19_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsenergylett.0c02629"},{"key":"e_1_2_7_20_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsenergylett.2c00099"},{"key":"e_1_2_7_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.201900784"},{"key":"e_1_2_7_22_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.2c17512"},{"key":"e_1_2_7_23_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-024-01619-2"},{"key":"e_1_2_7_24_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-020-0608-7"},{"key":"e_1_2_7_25_1","author":"Han 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