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While ferrocene is readily oxidised to the ferrocenium cation, higher oxidation states of uranocene are unknown. Here we report the elusive uranocenium cation, [U\n                    <jats:sup>V<\/jats:sup>\n                    (\u03b7\n                    <jats:sup>8<\/jats:sup>\n                    -C\n                    <jats:sub>8<\/jats:sub>\n                    H\n                    <jats:sub>8<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    ]\n                    <jats:sup>+<\/jats:sup>\n                    , and demonstrate using electron paramagnetic resonance spectroscopy and magnetometry that this formal U(V) complex has a 5\u2009\n                    <jats:italic>f<\/jats:italic>\n                    <jats:sup>1<\/jats:sup>\n                    ground state. Enhanced uranium 5\u2009\n                    <jats:italic>f<\/jats:italic>\n                    and 6\u2009\n                    <jats:italic>d<\/jats:italic>\n                    mixing into filled \u03b4-symmetry bonding orbitals in uranocenium, compared to uranocene, amplifies interorbital electron\u2013electron repulsion, and counteracts bond length contraction, which minimises structural change. This manifests in solution where the uranocene\/uranocenium redox couple exhibits near-ideal electrochemical reversibility, and in the solid-state where X-ray diffraction studies show minimal U\u2013C bond length change upon oxidation. This demonstrates a case where actinide covalency governs molecular structure and physical properties across both solid and solution phases.\n                  <\/jats:p>","DOI":"10.1038\/s41467-026-77066-2","type":"journal-article","created":{"date-parts":[[2026,10,23]],"date-time":"2026-10-23T09:01:41Z","timestamp":1792746101000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Isolation of uranocenium, the bis-[8]annulene uranium cation"],"prefix":"10.1038","volume":"17","author":[{"given":"Cameron N.","family":"Deakin","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-8907-7763","authenticated-orcid":false,"given":"Iulia","family":"Turcas","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Benjamin L. 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