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Herein, trifluoromethoxybenzene is proposed as a cosolvent for locally concentrated ionic liquid electrolytes (LCILEs) to reinforce the EEIs. With a comparative study of a neat ionic liquid electrolyte (ILE) and three LCILEs employing fluorobenzene, trifluoromethylbenzene, or trifluoromethoxybenzene as cosolvents, it is revealed that the fluorinated groups tethered to the benzene ring of the cosolvents not only affect the electrolytes\u2019 ionic conductivity and fluidity, but also the EEIs\u2019 composition via adjusting the contribution of the 1\u2010ethyl\u20103\u2010methylimidazolium cation (Emim<jats:sup>+<\/jats:sup>) and bis(fluorosulfonyl)imide anion. Trifluoromethoxybenzene, as the optimal cosolvent, leads to a stable cycling of LMBs employing 5 mAh cm<jats:sup>\u22122<\/jats:sup> lithium metal anodes (LMAs), 21\u00a0mg cm<jats:sup>\u22122<\/jats:sup> LiNi<jats:sub>0.8<\/jats:sub>Co<jats:sub>0.15<\/jats:sub>Al<jats:sub>0.05<\/jats:sub> (NCA) cathodes, and 4.2\u00a0\u00b5L mAh<jats:sup>\u22121<\/jats:sup> electrolytes for 150 cycles with a remarkable capacity retention of 71%, thanks to a solid electrolyte interphase rich in inorganic species on LMAs and, particularly, a uniform cathode\/electrolyte interphase rich in Emim<jats:sup>+<\/jats:sup>\u2010derived species on NCA cathodes. By contrast, the capacity retention under the same condition is only 16%, 46%, and 18% for the neat ILE and the LCILEs based on fluorobenzene and benzotrifluoride, respectively.<\/jats:p>","DOI":"10.1002\/adma.202309062","type":"journal-article","created":{"date-parts":[[2023,11,13]],"date-time":"2023-11-13T18:48:45Z","timestamp":1699901325000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":55,"title":["Reinforcing the Electrode\/Electrolyte Interphases of Lithium Metal Batteries Employing Locally Concentrated Ionic Liquid Electrolytes"],"prefix":"10.1002","volume":"36","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0532-316X","authenticated-orcid":false,"given":"Xu","family":"Liu","sequence":"first","affiliation":[{"name":"Helmholtz Institute Ulm (HIU)  Helmholtzstra\u00dfe 11 D\u201089081 Ulm Germany"},{"name":"Department of Chemistry and Biosciences Karlsruhe Institute of Technology (KIT) P.O. Box 3640 D\u201076021 Karlsruhe Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Alessandro","family":"Mariani","sequence":"additional","affiliation":[{"name":"ELETTRA Sincrotrone Trieste  Basovizza Trieste I\u201034012 Italy"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Thomas","family":"Diemant","sequence":"additional","affiliation":[{"name":"Helmholtz Institute Ulm (HIU)  Helmholtzstra\u00dfe 11 D\u201089081 Ulm Germany"},{"name":"Department of Chemistry and Biosciences Karlsruhe Institute of Technology (KIT) P.O. 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Box 3640 D\u201076021 Karlsruhe Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Andrea","family":"Mele","sequence":"additional","affiliation":[{"name":"Department of Chemistry Materials and Chemical Engineering \u201cGiulio Natta\u201d Politecnico di Milano  Piazza Leonardo da Vinci 32 Milan I\u201020133 Italy"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6606-5304","authenticated-orcid":false,"given":"Stefano","family":"Passerini","sequence":"additional","affiliation":[{"name":"Helmholtz Institute Ulm (HIU)  Helmholtzstra\u00dfe 11 D\u201089081 Ulm Germany"},{"name":"Department of Chemistry and Biosciences Karlsruhe Institute of Technology (KIT) P.O. Box 3640 D\u201076021 Karlsruhe Germany"},{"name":"Chemistry Department Sapienza University of Rome  Piazzale Aldo Moro 5 Rome I\u201000185 Italy"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2023,11,22]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41578-021-00345-5"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-019-0513-0"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.0c00275"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202004748"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-021-00792-y"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2021.12.018"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2019.02.004"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202216169"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202301312"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202219310"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202300443"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2021.06.014"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1EE02929K"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202207361"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1149\/2.0071906jes"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202219318"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202111360"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpcc.2c04503"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202003132"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202003752"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202207155"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ensm.2021.10.034"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202200862"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202003663"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202005991"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.2c06924"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1002\/batt.202100407"},{"key":"e_1_2_8_28_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ensm.2022.03.034"},{"key":"e_1_2_8_29_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202206648"},{"key":"e_1_2_8_30_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsenergylett.2c00232"},{"key":"e_1_2_8_31_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.201000052"},{"key":"e_1_2_8_32_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.coelec.2018.09.005"},{"key":"e_1_2_8_33_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202212446"},{"key":"e_1_2_8_34_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202301145"},{"key":"e_1_2_8_35_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.poly.2005.09.017"},{"key":"e_1_2_8_36_1","doi-asserted-by":"publisher","DOI":"10.1038\/ncomms12032"},{"key":"e_1_2_8_37_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202202405"},{"key":"e_1_2_8_38_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsenergylett.3c00052"},{"key":"e_1_2_8_39_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.molliq.2014.11.010"},{"key":"e_1_2_8_40_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.201702097"},{"key":"e_1_2_8_41_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202000520"},{"key":"e_1_2_8_42_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-023-36934-x"},{"key":"e_1_2_8_43_1","doi-asserted-by":"publisher","DOI":"10.1039\/C4CP03091E"},{"key":"e_1_2_8_44_1","volume-title":"Handbook of X\u2010Ray Photoelectron Spectroscopy","author":"Moulder J. 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