Hydrogenation of CO2 to MeOH Catalyzed by Highly Robust (PNNP)Ir Complexes Activated by Alkali Bases in Alcohol.
Inorg Chem
; 62(34): 14116-14123, 2023 Aug 28.
Article
em En
| MEDLINE
| ID: mdl-37589272
ABSTRACT
Despite receiving significant attention, well-defined homogeneous complexes for hydrogenation of carbon dioxide (CO2) to methanol (MeOH) are scarce and suffer issues of low catalyst turnover numbers (TONs) at high catalyst concentrations and deactivation in the presence of CO and at elevated temperatures. Herein, we disclose a system deploying sterically demanded (PNNP)Ir complexes for a sustained activity for hydrogenation of CO2 to MeOH at temperatures â¼200 °C in an alcohol solvent. Through reaction optimization, we achieved a TON of â¼9000 for MeOH formation, which exceeds most active homogeneous systems reported to date, and robustness on par with or exceeding most reactive systems utilizing amine additives was demonstrated. The key to achieving sustained catalyst turnover for the system was utilizing a catalytic amount of an alkali base additive, which serves the dual purpose of facilitating more efficient outer-sphere reduction of CO2 and HCO2Et and enhancing the selectivity of MeOH over in situ formed CO.
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Bases de dados:
MEDLINE
Idioma:
En
Revista:
Inorg Chem
Ano de publicação:
2023
Tipo de documento:
Article
País de afiliação:
Japão