Fast CO2 hydrogenation to formic acid catalyzed by an Ir(PSiP) pincer hydride in a DMSO/water/ionic liquid solvent system
Complex [IrClH{κP,P,Si-Si(Me)(C6H4–2-PiPr2)2}] (1) showed a remarkable catalytic activity for CO2 hydrogenation in a DMSO/H2O solvent system incorporating 1,2-dimethyl-3-butylimidazolium acetate ionic liquid (IL), producing 0.94 M formic acid with initial TOFs up to 1432 h−1 (CO2/H2 = 20/40 bar, 30...
| Autores: | , , , , , |
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| Tipo de documento: | artigo |
| Estado: | Versão publicada |
| Data de publicação: | 2020 |
| País: | España |
| Recursos: | Consejo Superior de Investigaciones Científicas (CSIC) |
| Repositório: | DIGITAL.CSIC. Repositorio Institucional del CSIC |
| OAI Identifier: | oai:digital.csic.es:10261/233103 |
| Acesso em linha: | http://hdl.handle.net/10261/233103 |
| Access Level: | Acceso aberto |
| Palavra-chave: | Ionic liquids Solvent-cage CO2 hydrogenation Formic acid Iridium |
| Resumo: | Complex [IrClH{κP,P,Si-Si(Me)(C6H4–2-PiPr2)2}] (1) showed a remarkable catalytic activity for CO2 hydrogenation in a DMSO/H2O solvent system incorporating 1,2-dimethyl-3-butylimidazolium acetate ionic liquid (IL), producing 0.94 M formic acid with initial TOFs up to 1432 h−1 (CO2/H2 = 20/40 bar, 30 °C). While the hydrogenation outcome followed dependences upon gas composition, pressure and temperature similar to those of other efficient systems in DMSO/H2O, the kinetic dependence upon catalyst loading revealed non-linear effects suggestive of relevant IL-catalyst interactions. NMR speciation studies identified two major complexes, [Ir(OCHO)(H){κP,P,Si-Si(Me)(C6H4–2-PiPr2)2}] (2) and [Ir(H)2{κP,P,Si-Si(Me)(C6H4–2-PiPr2)2}(DMSO)] (3), potentially responsible for catalytic cycling though inactive outside the current solvent system. |
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