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With the ever\u2010increasing projections for electric vehicles, the dependency of current Li\u2010ion batteries on the ever\u2010fluctuating cobalt prices poses serious environmental and sustainability issues. To address these challenges, a new class of cobalt\u2010free materials with general formula of LiNi<jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>Fe<jats:italic><jats:sub>y<\/jats:sub><\/jats:italic>Al<jats:italic><jats:sub>z<\/jats:sub><\/jats:italic>O<jats:sub>2<\/jats:sub> (<jats:italic>x<\/jats:italic> + <jats:italic>y<\/jats:italic> + <jats:italic>z<\/jats:italic> = 1), termed as the lithium iron aluminum nickelate (NFA) class of cathodes, is introduced. These cobalt\u2010free materials are synthesized using the sol\u2013gel process to explore their compositional landscape by varying aluminum and iron. These NFA variants are characterized using electron microscopy, neutron and X\u2010ray diffraction, and M\u00f6ssbauer and X\u2010ray photoelectron spectroscopy to investigate their morphological, physical, and crystal\u2010structure properties. Operando experiments by X\u2010ray diffraction, M\u00f6ssbauer spectroscopy, and galvanostatic intermittent titration have been also used to study the crystallographic transitions, electrochemical activity, and Li\u2010ion diffusivity upon lithium removal and uptake in the NFA cathodes. NFA compositions yield specific capacities of \u2248200 mAh g<jats:sup>\u22121<\/jats:sup>, demonstrating reasonable rate capability and cycling stability with \u224880% capacity retention after 100 charge\/discharge cycles. While this is an early stage of research, the potential that these cathodes could have as viable candidates in next\u2010generation cobalt\u2010free lithium\u2010ion batteries is highlighted here.<\/jats:p>","DOI":"10.1002\/adma.202002960","type":"journal-article","created":{"date-parts":[[2020,7,16]],"date-time":"2020-07-16T02:56:16Z","timestamp":1594868176000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":111,"title":["Lithium Iron Aluminum Nickelate, LiNi<i><sub>x<\/sub><\/i>Fe<i><sub>y<\/sub><\/i>Al<i><sub>z<\/sub><\/i>O<sub>2<\/sub>\u2014New Sustainable Cathodes for Next\u2010Generation Cobalt\u2010Free Li\u2010Ion Batteries"],"prefix":"10.1002","volume":"32","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-6042-5295","authenticated-orcid":false,"given":"Nitin","family":"Muralidharan","sequence":"first","affiliation":[{"name":"Energy and Transportation Science Division Oak Ridge National Laboratory  Oak Ridge TN 37830 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