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This concept is feasible due to the selective enrichment of redox organic molecules in each aqueous phase of ABS, which spontaneously form two liquid\u2010phases above given concentrations of salt and IL. Therefore, the required separation of electrolytes in the battery is not driven by an expensive membrane that hampers mass transfer, but instead, by the intrinsic immiscibility of the two liquid phases. Moreover, the crosscontamination typically occurring through the ineffective membranes is determined by the partition coefficients of the active molecules between the two phases. The phase diagrams of a series of IL\u2010based ABS are characterized, the partition coefficients of several redox organic molecules are determined, and the electrochemistry of these redox\u2010active immiscible phases is evaluated, allowing appraisal of the battery performance. Several redox ABS that may be used in total aqueous membrane\u2010free batteries with theoretical battery voltages as high as 1.6 V are identified. The viability of a membrane\u2010free battery composed of an IL\u2010based ABS containing methyl viologen and 2,2,6,6\u2010tetramethyl\u20101\u2010piperidinyloxy as active species is demonstrated.<\/jats:p>","DOI":"10.1002\/advs.201800576","type":"journal-article","created":{"date-parts":[[2018,8,9]],"date-time":"2018-08-09T00:10:19Z","timestamp":1533773419000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":67,"title":["Pioneering Use of Ionic Liquid\u2010Based Aqueous Biphasic Systems as Membrane\u2010Free Batteries"],"prefix":"10.1002","volume":"5","author":[{"given":"Paula","family":"Navalpotro","sequence":"first","affiliation":[{"name":"Electrochemical Processes Unit IMDEA Energy Institute  Avda. Ram\u00f3n de la Sagra 3 28935 M\u00f3stoles Spain"}]},{"given":"Catarina M. S. S.","family":"Neves","sequence":"additional","affiliation":[{"name":"CICECO \u2010 Aveiro Institute of Materials Chemistry Department University of Aveiro  3810\u2010193 Aveiro Portugal"}]},{"given":"Jesus","family":"Palma","sequence":"additional","affiliation":[{"name":"Electrochemical Processes Unit IMDEA Energy Institute  Avda. Ram\u00f3n de la Sagra 3 28935 M\u00f3stoles Spain"}]},{"given":"Mara G.","family":"Freire","sequence":"additional","affiliation":[{"name":"CICECO \u2010 Aveiro Institute of Materials Chemistry Department University of Aveiro  3810\u2010193 Aveiro Portugal"}]},{"given":"Jo\u00e3o A. P.","family":"Coutinho","sequence":"additional","affiliation":[{"name":"CICECO \u2010 Aveiro Institute of Materials Chemistry Department University of Aveiro  3810\u2010193 Aveiro Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5660-6381","authenticated-orcid":false,"given":"Rebeca","family":"Marcilla","sequence":"additional","affiliation":[{"name":"Electrochemical Processes Unit IMDEA Energy Institute  Avda. 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