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Layered K\u2010metal oxides have too high a voltage slope due to their large K<jats:sup>+<\/jats:sup>\u2013K<jats:sup>+<\/jats:sup> interaction, resulting in low specific capacity and average voltage. In contrast, the 3D arrangement of K<jats:sup>+<\/jats:sup>, with polyanions separating them, reduces the strength of the effective K<jats:sup>+<\/jats:sup>\u2010K<jats:sup>+<\/jats:sup> repulsion, which in turn increases specific capacity and voltage. Here, stoichiometric KVPO<jats:sub>4<\/jats:sub>F for use as a high\u2010energy\u2010density K\u2010ion cathode is developed. The KVPO<jats:sub>4<\/jats:sub>F cathode delivers a reversible capacity of \u2248105 mAh g<jats:sup>\u22121<\/jats:sup> with an average voltage of \u22484.3 V (vs K\/K<jats:sup>+<\/jats:sup>), resulting in a gravimetric energy density of \u2248450 Wh kg<jats:sup>\u22121<\/jats:sup>. During electrochemical cycling, the K<jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>VPO<jats:sub>4<\/jats:sub>F cathode goes through various intermediate phases at <jats:italic>x<\/jats:italic> = 0.75, 0.625, and 0.5 upon K extraction and reinsertion, as determined by ex situ X\u2010ray diffraction characterization and ab initio calculations. This work further explains the role of oxygen substitution in KVPO<jats:sub>4+<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>F<jats:sub>1\u2212<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>: the oxygenation of KVPO<jats:sub>4<\/jats:sub>F leads to an anion\u2010disordered structure which prevents the formation of K<jats:sup>+<\/jats:sup>\/vacancy orderings without electrochemical plateaus and hence to a smoother voltage profile.<\/jats:p>","DOI":"10.1002\/aenm.201801591","type":"journal-article","created":{"date-parts":[[2018,7,18]],"date-time":"2018-07-18T22:55:03Z","timestamp":1531954503000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":183,"title":["A New Strategy for High\u2010Voltage Cathodes for K\u2010Ion Batteries: Stoichiometric KVPO<sub>4<\/sub>F"],"prefix":"10.1002","volume":"8","author":[{"given":"Haegyeom","family":"Kim","sequence":"first","affiliation":[{"name":"Materials Sciences Division Lawrence Berkeley National Laboratory  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dong\u2010Hwa","family":"Seo","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering University of California  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Matteo","family":"Bianchini","sequence":"additional","affiliation":[{"name":"Materials Sciences Division Lawrence Berkeley National Laboratory  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rapha\u00eble J.","family":"Cl\u00e9ment","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering University of California  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hyunchul","family":"Kim","sequence":"additional","affiliation":[{"name":"Materials Sciences Division Lawrence Berkeley National Laboratory  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jae Chul","family":"Kim","sequence":"additional","affiliation":[{"name":"Materials Sciences Division Lawrence Berkeley National Laboratory  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yaosen","family":"Tian","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering University of California  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tan","family":"Shi","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering University of California  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Won\u2010Sub","family":"Yoon","sequence":"additional","affiliation":[{"name":"Department of Energy Science Sungkyunkwan University  Suwon 16419 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9275-3605","authenticated-orcid":false,"given":"Gerbrand","family":"Ceder","sequence":"additional","affiliation":[{"name":"Materials Sciences Division Lawrence Berkeley National Laboratory  Berkeley CA 94720 USA"},{"name":"Department of Materials Science and Engineering University of California  Berkeley CA 94720 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2018,7,18]]},"reference":[{"key":"e_1_2_8_1_1","volume-title":"The Economist","author":"Atacama S. 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