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Ti and Zr amino-tris(phenolate) catalysts for the synthesis of cyclic carbonates from CO_(2) and epoxides

Green Chemical Engineering 2022年第2期3卷 171-179页

作者： Aeilke J.Kamphuis Minhhuy Tran Francesco picchioni paolo p.pescarmona Chemical Engineering Group Engineering and Technology Institute Groningen(ENTEG)Faculty of Science and EngineeringUniversity of GroningenNijenborgh 49747AGGroningenthe Netherlands

Herein,we report the application of four amino-tris(phenolate)-based metal complexes incorporating Ti(IV)or Zr(IV)centres(2a-3b)as homogeneous catalysts for the conversion of CO_(2)and epoxides into cyclic *** four complexes were synthesised,characterised and then evaluated in combination with tetrabutylammo-nium iodide,bromide or chloride as binary catalytic systems for the reaction of CO_(2)with 1,2-epoxyhexane as epoxide substrate at 12 bar CO_(2)pressure and 90?C for 2 *** catalytic systems comprising the two Ti(IV)complexes(2a and 2b)showed similar *** notable exception was the catalytic system consisting of titanium complex 2b,bearing an axial Cl-ligand,and tetrabutylammonium chloride,which displayed higher catalytic activity compared to other titanium-based *** higher activity was achieved with Zr(IV)complex 3a,bearing an axial isopropoxide ligand,which reached turnover numbers(TON metal)up to 1920 for the reaction of CO_(2)with 1,2-epoxyhexane at 12 bar CO_(2)pressure and 90?C for 2 *** performance is comparable with that of state-of-the-art catalysts for this *** catalytic system consisting of complex 3a and tetra-butylammonium bromide was explored further by investigating its applicability with a broad substrate scope,achieving quantitative conversion of several epoxides with CO_(2)into cyclic carbonate products at 90?C and 12 bar CO_(2)pressure for 18 *** selectivity towards the cyclic carbonate products was?98%for all studied terminal epoxides and?80%for all examined cyclohexene-type epoxides.

关键词： CO_(2)fixation Cyclic carbonates Homogeneous catalysis Ti amino-tris(phenolate)complexes Zr amino-tris(phenolate)complexes

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