Journal
ACS CATALYSIS
Volume 9, Issue 10, Pages 9317-9326Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b02280
Keywords
carbon dioxide; acid-assisted ester hydrogenation; cascade catalysis; carbon dioxide to methanol; Lewis acid catalyst
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Funding
- NSF through the CCI Center for Enabling New Technologies through Catalysis (CENTC) Phase II Renewal [CHE-1205189]
- Vagelos Institute for Energy Science and Technology at the University of Pennsylvania
- NSF Graduate Research Fellowship Program [DGE-1256082]
- Vagelos Integrated Program in Energy Research (VIPER) at the University of Pennsylvania
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A catalytic cascade system for CO2 hydrogenation to MeOH under acidic conditions is described. The reaction uses three catalysts which promote stepwise formation and conversion of formic acid and formate ester intermediates. The activities and decomposition pathways of different catalyst candidates for each step were investigated. The combination Ru(H)(2)[P(CH2CH2PPh2)(3)]/Sc(OTf)(3)/Ir(tBuPCP)(CO) was found to be the most active for CO2 hydrogenation to MeOH. An overall TON of 428 was achieved after 40 h at 155 degrees C in EtOH, resulting in a high concentration of MeOH (1.07 M). Catalyst speciation studies upon completion of the reaction indicated that the carbonyl complexes [Ru[P(CH3CH2PPh2)(3)](H)(CO)](OTf), Ir(tBuPCP)(H)(CO)(OTf), and [Ir(tBuPCP)(H)(CO)(2)](OTf) were formed as the major metal-containing species. Notably, [Ru[P(CH3CH2PPh2)(3)](H)(CO)](OTf) was found to be inactive for CO2 hydrogenation, limiting the productivity of the reaction.
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