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However, carbonate electrolytes form unstable interphases, hindering their practical implementation. Alternatively, fluorinated sulfonylimide (FSI\n                    <jats:sup>\u2212<\/jats:sup>\n                    \/TFSI\n                    <jats:sup>\u2212<\/jats:sup>\n                    ) based ionic liquid (IL) electrolytes, coupled with Li\u2010imide salts, enable anion\u2010derived SEI formation, thereby enhancing capacity retention. However, the functional role of these anions in directing SEI formation and evolution within IL\u2010based systems is poorly understood. Moreover, the mechanistic interplay between the decomposition pathways of symmetric and asymmetric anions in governing interfacial chemistry remains elusive. Herein, we investigate the chemistry and morphology of SEIs formed using various imidazolium\u2010based ILs containing both symmetric and asymmetric anions. We reveal that the synergistic interactions between symmetrical bis(fluorinated sulfonyl)imide anions and imidazolium cations facilitate an inorganic\u2010rich (LiF\/LiOH) inner and a Li\n                    <jats:sub>2<\/jats:sub>\n                    SO\n                    <jats:sub>4<\/jats:sub>\n                    \/polymeric outer layer SEI, conformally coating the 3D Si interface. The complementary effects of inorganic\u2010rich and polymer components, featuring key Li\n                    <jats:sub>2<\/jats:sub>\n                    SO\n                    <jats:sub>4<\/jats:sub>\n                    species, reinforce mechanical integrity and flexibility, suppressing pulverization and enabling reversible capacity of 2489\u00a0mAh\/g at 1C over 250 cycles. Correlating electrochemical performance with surface analysis provides critical insights into the impact of fluorinated sulfonylimide on passivation behavior and battery performance, guiding future design of ionic liquid electrolytes for LIBs.\n                  <\/jats:p>","DOI":"10.1002\/anie.202522709","type":"journal-article","created":{"date-parts":[[2025,12,2]],"date-time":"2025-12-02T07:14:46Z","timestamp":1764659686000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Symmetric Vs Asymmetric Imide Anion Decomposition Pathways And Their Influence On Solid Electrolyte Interphase Stability For Si Anodes"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-8651-7304","authenticated-orcid":false,"given":"Abinaya","family":"Sankaran","sequence":"first","affiliation":[{"name":"Department of Chemical Sciences and Bernal Institute University of Limerick  Castletroy Limerick V94T9PX Ireland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fathima","family":"Laffir","sequence":"additional","affiliation":[{"name":"Department of Chemical Sciences and Bernal Institute University of Limerick  Castletroy Limerick V94T9PX Ireland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Giovanna","family":"Maresca","sequence":"additional","affiliation":[{"name":"Technologies and Devices for Electrochemical Storage (TERIN\u2010DEC\u2010ACEL) Technical Unit ENEA (Italian National Agency for New Technology, Energy and Sustainable Economic Development)  Rome 00123 Italy"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nilotpal","family":"Kapuria","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indiana University \u2212Bloomington  Bloomington Indiana 47405 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Marc","family":"Van der Velden","sequence":"additional","affiliation":[{"name":"Smit Thermal Solutions B.V.  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