Iridium Complexes with Proton-Responsive Azole-Type Ligands as Effective Catalysts for CO2 Hydrogenation
Abstract
Abstract Pentamethylcyclopentadienyl iridium (Cp*Ir) complexes with bidentate ligands consisting of a pyridine ring and an electron‐rich diazole ring were prepared. Their catalytic activity toward CO 2 hydrogenation in 2.0 m KHCO 3 aqueous solutions (pH 8.5) at 50 °C, under 1.0 MPa CO 2 /H 2 (1:1) have been reported as an alternative to photo‐ and electrochemical CO 2 reduction. Bidentate ligands incorporating an electron‐rich diazole ring improved the catalytic performance of the Ir complexes compared to the bipyridine ligand. Complexes 2 , 4 , and 6 , possessing both a hydroxy group and an uncoordinated NH group, which are proton‐responsive and capable of generating pendent bases in basic media, recorded high initial turnover frequency values of 1300, 1550, and 2000 h −1 , respectively. Spectroscopic and computational investigations revealed that the reversible deprotonation changes the electronic properties of the complexes and causes interactions between pendent base and substrate and/or solvent water molecules, resulting in high catalytic performance in basic media.
- Authors:
-
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- National Institute of Advanced Industrial Science and Technology, Ibaraki (Japan)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1405934
- Alternate Identifier(s):
- OSTI ID: 1407830
- Report Number(s):
- BNL-114435-2017-JA
Journal ID: ISSN 1864-5631; R&D Project: CO026; KC0304030; TRN: US1702901
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemSusChem
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 22; Journal ID: ISSN 1864-5631
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 hydrogenation formic acid catalysis iridium DFT
Citation Formats
Ertem, Mehmed Zahid, Suna, Yuki, Himeda, Yuichiro, Muckerman, James T., and Fujita, Etsuko. Iridium Complexes with Proton-Responsive Azole-Type Ligands as Effective Catalysts for CO2 Hydrogenation. United States: N. p., 2017.
Web. doi:10.1002/cssc.201701676.
Ertem, Mehmed Zahid, Suna, Yuki, Himeda, Yuichiro, Muckerman, James T., & Fujita, Etsuko. Iridium Complexes with Proton-Responsive Azole-Type Ligands as Effective Catalysts for CO2 Hydrogenation. United States. https://doi.org/10.1002/cssc.201701676
Ertem, Mehmed Zahid, Suna, Yuki, Himeda, Yuichiro, Muckerman, James T., and Fujita, Etsuko. Fri .
"Iridium Complexes with Proton-Responsive Azole-Type Ligands as Effective Catalysts for CO2 Hydrogenation". United States. https://doi.org/10.1002/cssc.201701676. https://www.osti.gov/servlets/purl/1405934.
@article{osti_1405934,
title = {Iridium Complexes with Proton-Responsive Azole-Type Ligands as Effective Catalysts for CO2 Hydrogenation},
author = {Ertem, Mehmed Zahid and Suna, Yuki and Himeda, Yuichiro and Muckerman, James T. and Fujita, Etsuko},
abstractNote = {Abstract Pentamethylcyclopentadienyl iridium (Cp*Ir) complexes with bidentate ligands consisting of a pyridine ring and an electron‐rich diazole ring were prepared. Their catalytic activity toward CO 2 hydrogenation in 2.0 m KHCO 3 aqueous solutions (pH 8.5) at 50 °C, under 1.0 MPa CO 2 /H 2 (1:1) have been reported as an alternative to photo‐ and electrochemical CO 2 reduction. Bidentate ligands incorporating an electron‐rich diazole ring improved the catalytic performance of the Ir complexes compared to the bipyridine ligand. Complexes 2 , 4 , and 6 , possessing both a hydroxy group and an uncoordinated NH group, which are proton‐responsive and capable of generating pendent bases in basic media, recorded high initial turnover frequency values of 1300, 1550, and 2000 h −1 , respectively. Spectroscopic and computational investigations revealed that the reversible deprotonation changes the electronic properties of the complexes and causes interactions between pendent base and substrate and/or solvent water molecules, resulting in high catalytic performance in basic media.},
doi = {10.1002/cssc.201701676},
journal = {ChemSusChem},
number = 22,
volume = 10,
place = {United States},
year = {Fri Oct 06 00:00:00 EDT 2017},
month = {Fri Oct 06 00:00:00 EDT 2017}
}
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