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The structures of the complexes were studied by X\u2010ray diffraction and multinuclear NMR spectroscopy. We found that the cerium(III) ion can induce the elimination of one of the <jats:italic>i<\/jats:italic>Pr groups at phosphorus to yield a new dianionic PNP tridentate framework (PNP<jats:sup>\u2010<jats:italic>i<\/jats:italic>Pr<\/jats:sup>) featuring a phosphido\u2010donor functionality, which is bound to the cerium ion with the shortest known Ce\u2212P bond of 2.7884(14)\u2005\u00c5 for molecular compounds. The reaction of the complex [(PNP)Ce{N(SiMe<jats:sub>3<\/jats:sub>)<jats:sub>2<\/jats:sub>}<jats:sub>2<\/jats:sub>]\u2005(<jats:bold>1<\/jats:bold>) with Ph<jats:sub>2<\/jats:sub>CO gave the Ce\u2010bound product of C\u2212C coupling, <jats:sup>\u2010<\/jats:sup>N(SiMe<jats:sub>3<\/jats:sub>)SiMe<jats:sub>2<\/jats:sub>CH<jats:sub>2<\/jats:sub>\u2010CPh<jats:sub>2<\/jats:sub>O<jats:sup>\u2212<\/jats:sup>, through the C\u2212H bond activation of a SiMe<jats:sub>3<\/jats:sub> group. <jats:sup>31<\/jats:sup>P\u2005NMR spectroscopy was used to estimate the presence of a vacant coordination position at the cerium ion in the Ce<jats:sup>III<\/jats:sup>\u2013PNP complexes by the examination of the <jats:italic>\u03b4<\/jats:italic>(<jats:sup>31<\/jats:sup>P) shift recorded both in non\u2010polar (C<jats:sub>6<\/jats:sub>D<jats:sub>6<\/jats:sub>) and polar ([D<jats:sub>8<\/jats:sub>]THF) solvents. Moreover, <jats:sup>31<\/jats:sup>P\u2005NMR spectroscopy was also found to be a useful tool for the estimation of the Ce\u2212P bond distances in {(PNP)Ce<jats:sup>III<\/jats:sup>} and {(PNP)<jats:sub>2<\/jats:sub>Ce<jats:sup>III<\/jats:sup>} systems. Electrochemical and computational studies for <jats:bold>1<\/jats:bold> and its lanthanum analogue containing a redox\u2010innocent metal center revealed the stabilization of the Ce<jats:sup>III<\/jats:sup> oxidation state by the PNP ligand.<\/jats:p>","DOI":"10.1002\/chem.201703174","type":"journal-article","created":{"date-parts":[[2017,8,10]],"date-time":"2017-08-10T22:26:42Z","timestamp":1502404002000},"page":"17923-17934","source":"Crossref","is-referenced-by-count":24,"title":["Structure, Electronics and Reactivity of Ce(PNP) Complexes"],"prefix":"10.1002","volume":"23","author":[{"given":"Alexander V.","family":"Zabula","sequence":"first","affiliation":[{"name":"P. Roy and Diana T. 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