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The [Ln(OSi(OtBu)<jats:sub>3<\/jats:sub>)<jats:sub>4<\/jats:sub>K<jats:sub>2<\/jats:sub>] complexes (Ln=Eu, Yb) are stable at room temperature, but they promote the reduction of azobenzene to yield the KPhNNPh radical anion as well as the reductive cleavage of CS<jats:sub>2<\/jats:sub> to yield CS<jats:sub>3<\/jats:sub><jats:sup>2\u2212<\/jats:sup> as the major product. The Eu<jats:sup>III<\/jats:sup> complex of the radical anion PhNNPh is structurally characterized. Moreover, [Yb(OSi(OtBu)<jats:sub>3<\/jats:sub>)<jats:sub>4<\/jats:sub>K<jats:sub>2<\/jats:sub>] can reduce CO<jats:sub>2<\/jats:sub> at room temperature. Release of the reduction products in D<jats:sub>2<\/jats:sub>O shows the quantitative formation of both oxalate and carbonate in a 1:2.2 ratio. The bulky siloxide ligands enforce the labile binding of the reduction products providing the opportunity to establish a closed synthetic cycle for the Yb<jats:sup>II<\/jats:sup>\u2010mediated CO<jats:sub>2<\/jats:sub> reduction. These studies show that the presence of four electron\u2010rich siloxide ligands renders their Eu<jats:sup>II<\/jats:sup> and Yb<jats:sup>II<\/jats:sup> complexes highly reactive.<\/jats:p>","DOI":"10.1002\/anie.201405031","type":"journal-article","created":{"date-parts":[[2014,7,31]],"date-time":"2014-07-31T00:47:46Z","timestamp":1406767666000},"page":"10448-10452","source":"Crossref","is-referenced-by-count":63,"title":["Tuning Lanthanide Reactivity Towards Small Molecules with Electron\u2010Rich Siloxide Ligands"],"prefix":"10.1002","volume":"53","author":[{"given":"Julie","family":"Andrez","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jacques","family":"P\u00e9caut","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pierre\u2010Alain","family":"Bayle","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Marinella","family":"Mazzanti","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2014,7,30]]},"reference":[{"key":"e_1_2_2_1_2","doi-asserted-by":"publisher","DOI":"10.1002\/3527609350"},{"key":"e_1_2_2_2_2","unstructured":"\u00a0"},{"key":"e_1_2_2_3_2","first-page":"303","volume-title":"Progress in Inorganic Chemistry","author":"Pierre H. 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