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The uranium(V) nitride [U(Tren<jats:sup>TIPS<\/jats:sup>)(N)][K(B15C5)<jats:sub>2<\/jats:sub>] (<jats:bold>1<\/jats:bold>, Tren<jats:sup>TIPS<\/jats:sup>=N(CH<jats:sub>2<\/jats:sub>CH<jats:sub>2<\/jats:sub>NSi<jats:italic>i<\/jats:italic>Pr<jats:sub>3<\/jats:sub>)<jats:sub>3<\/jats:sub>; B15C5=benzo\u201015\u2010crown\u20105) reacts with CO<jats:sub>2<\/jats:sub> to give [U(Tren<jats:sup>TIPS<\/jats:sup>)(O)(NCO)][K(B15C5)<jats:sub>2<\/jats:sub>] (<jats:bold>3<\/jats:bold>), whereas the uranium(VI) nitride [U(Tren<jats:sup>TIPS<\/jats:sup>)(N)] (<jats:bold>2<\/jats:bold>) reacts with CO<jats:sub>2<\/jats:sub> to give isolable [U(Tren<jats:sup>TIPS<\/jats:sup>)(O)(NCO)] (<jats:bold>4<\/jats:bold>); complex <jats:bold>4<\/jats:bold> rapidly decomposes to known [U(Tren<jats:sup>TIPS<\/jats:sup>)(O)] (<jats:bold>5<\/jats:bold>) with concomitant formation of N<jats:sub>2<\/jats:sub> and CO proposed, with the latter trapped as a vanadocene adduct. In contrast, <jats:bold>1<\/jats:bold> reacts with CS<jats:sub>2<\/jats:sub> to give [U(Tren<jats:sup>TIPS<\/jats:sup>)(\u03ba<jats:sup>2<\/jats:sup>\u2010CS<jats:sub>3<\/jats:sub>)][K(B15C5)<jats:sub>2<\/jats:sub>] (<jats:bold>6<\/jats:bold>), <jats:bold>2<\/jats:bold>, and [K(B15C5)<jats:sub>2<\/jats:sub>][NCS] (<jats:bold>7<\/jats:bold>), whereas <jats:bold>2<\/jats:bold> reacts with CS<jats:sub>2<\/jats:sub> to give [U(Tren<jats:sup>TIPS<\/jats:sup>)(NCS)] (<jats:bold>8<\/jats:bold>) and \u201cS\u201d, with the latter trapped as Ph<jats:sub>3<\/jats:sub>PS. Calculated reaction profiles reveal outer\u2010sphere reactivity for uranium(V) but inner\u2010sphere mechanisms for uranium(VI); despite the wide divergence of products the initial activation of CE<jats:sub>2<\/jats:sub> follows mechanistically related pathways, providing insight into the factors of uranium oxidation state, chalcogen, and NCE groups that govern the subsequent divergent redox reactions that include common one\u2010electron reactions and a less\u2010common two\u2010electron redox event. Caution, we suggest, is warranted when utilising CS<jats:sub>2<\/jats:sub> as a reactivity surrogate for CO<jats:sub>2<\/jats:sub>.<\/jats:p>","DOI":"10.1002\/chem.201605620","type":"journal-article","created":{"date-parts":[[2017,1,11]],"date-time":"2017-01-11T10:47:25Z","timestamp":1484131645000},"page":"2950-2959","source":"Crossref","is-referenced-by-count":43,"title":["Terminal Uranium(V\/VI) Nitride Activation of Carbon Dioxide and Carbon Disulfide: Factors Governing Diverse and Well\u2010Defined Cleavage and Redox Reactions"],"prefix":"10.1002","volume":"23","author":[{"given":"Peter A.","family":"Cleaves","sequence":"first","affiliation":[{"name":"School of Chemistry The University of Manchester  Oxford Road Manchester M13 9PL UK"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Christos E.","family":"Kefalidis","sequence":"additional","affiliation":[{"name":"LPCNO, CNRS &amp; INSA Universit\u00e9 Paul Sabatier  135 Avenue de Rangueil Toulouse 31077 France"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Benedict M.","family":"Gardner","sequence":"additional","affiliation":[{"name":"School of Chemistry The University of Manchester  Oxford Road Manchester M13 9PL UK"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Floriana","family":"Tuna","sequence":"additional","affiliation":[{"name":"School of Chemistry and Photon Science Institute The University of Manchester  Oxford Road Manchester M13 9PL UK"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Eric J. 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