Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 14, Pages 5830-5836Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201916483
Keywords
carbon dioxide; cerium; cycloaddition; epoxides; pyrazolates
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The homoleptic pyrazolate complexes [Ce-4(III)(Me(2)pz)(12)] and [Ce-IV(Me(2)pz)(4)](2) quantitatively insert CO2 to give [Ce-4(III)(Me(2)pzCO(2))(12)] and [Ce-IV(Me(2)pzCO(2))(4)], respectively (Me(2)pz=3,5-dimethylpyrazolato). This process is reversible for both complexes, as observed by in situ IR and NMR spectroscopy in solution and by TGA in the solid state. By adjusting the molar ratio, one molecule of CO2 per [Ce-IV(Me(2)pz)(4)] complex could be inserted to give trimetallic [Ce-3(Me(2)pz)(9)(Me(2)pzCO(2))(3)(thf)]. Both the cerous and ceric insertion products catalyze the formation of cyclic carbonates from epoxides and CO2 under mild conditions. In the absence of epoxide, the ceric catalyst is prone to reduction by the co-catalyst tetra-n-butylammonium bromide (TBAB).
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