Highly robust hydrogen generation by bio-inspired Ir complexes for dehydrogenation of formic acid in water: Experimental and theoretical mechanistic investigations at different pH
Abstract
Hydrogen generation from formic acid (FA), one of the most promising hydrogen storage materials, has attracted much attention due to the demand for the development of renewable energy carriers. Catalytic dehydrogenation of FA in an efficient and green manner remains challenging. Here, we report a series of bio-inspired Ir complexes for highly robust and selective hydrogen production from FA in aqueous solutions without organic solvents or additives. One of these complexes bearing an imidazoline moiety (complex 6) achieved a turnover frequency (TOF) of 322,000 h⁻¹ at 100 °C, which is higher than ever reported. The novel catalysts are very stable and applicable in highly concentrated FA. For instance, complex 3 (1 μmol) affords an unprecedented turnover number (TON) of 2,050,000 at 60 °C. Deuterium kinetic isotope effect experiments and density functional theory (DFT) calculations employing a “speciation” approach demonstrated a change in the rate-determining step with increasing solution pH. This study provides not only more insight into the mechanism of dehydrogenation of FA but also offers a new principle for the design of effective homogeneous organometallic catalysts for H₂ generation from FA.
- Authors:
-
- Dalian Univ. of Technology, Panjin (China)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- National Institute of Advanced Industrial Science and Technology, Ibaraki (Japan)
- National Institute of Advanced Industrial Science and Technology, Ibaraki (Japan); Japan Science and Technology Agency, Saitama (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:
- 1213386
- Report Number(s):
- BNL-108268-2015-JA
Journal ID: ISSN 2155-5435; R&D Project: CO026; KC0304030
- Grant/Contract Number:
- SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 36; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; formic acid dehydrogenation; Ir complexes; mechanism; kinetic isotope effect; pH-dependence
Citation Formats
Wang, Wan -Hui, Fujita, Etsuko, Ertem, Mehmed Z., Xu, Shaoan, Onishi, Naoya, Manaka, Yuichi, Suna, Yuki, Kambayashi, Hide, Muckerman, James T., and Himeda, Yuichiro. Highly robust hydrogen generation by bio-inspired Ir complexes for dehydrogenation of formic acid in water: Experimental and theoretical mechanistic investigations at different pH. United States: N. p., 2015.
Web. doi:10.1021/acscatal.5b01090.
Wang, Wan -Hui, Fujita, Etsuko, Ertem, Mehmed Z., Xu, Shaoan, Onishi, Naoya, Manaka, Yuichi, Suna, Yuki, Kambayashi, Hide, Muckerman, James T., & Himeda, Yuichiro. Highly robust hydrogen generation by bio-inspired Ir complexes for dehydrogenation of formic acid in water: Experimental and theoretical mechanistic investigations at different pH. United States. https://doi.org/10.1021/acscatal.5b01090
Wang, Wan -Hui, Fujita, Etsuko, Ertem, Mehmed Z., Xu, Shaoan, Onishi, Naoya, Manaka, Yuichi, Suna, Yuki, Kambayashi, Hide, Muckerman, James T., and Himeda, Yuichiro. Thu .
"Highly robust hydrogen generation by bio-inspired Ir complexes for dehydrogenation of formic acid in water: Experimental and theoretical mechanistic investigations at different pH". United States. https://doi.org/10.1021/acscatal.5b01090. https://www.osti.gov/servlets/purl/1213386.
@article{osti_1213386,
title = {Highly robust hydrogen generation by bio-inspired Ir complexes for dehydrogenation of formic acid in water: Experimental and theoretical mechanistic investigations at different pH},
author = {Wang, Wan -Hui and Fujita, Etsuko and Ertem, Mehmed Z. and Xu, Shaoan and Onishi, Naoya and Manaka, Yuichi and Suna, Yuki and Kambayashi, Hide and Muckerman, James T. and Himeda, Yuichiro},
abstractNote = {Hydrogen generation from formic acid (FA), one of the most promising hydrogen storage materials, has attracted much attention due to the demand for the development of renewable energy carriers. Catalytic dehydrogenation of FA in an efficient and green manner remains challenging. Here, we report a series of bio-inspired Ir complexes for highly robust and selective hydrogen production from FA in aqueous solutions without organic solvents or additives. One of these complexes bearing an imidazoline moiety (complex 6) achieved a turnover frequency (TOF) of 322,000 h⁻¹ at 100 °C, which is higher than ever reported. The novel catalysts are very stable and applicable in highly concentrated FA. For instance, complex 3 (1 μmol) affords an unprecedented turnover number (TON) of 2,050,000 at 60 °C. Deuterium kinetic isotope effect experiments and density functional theory (DFT) calculations employing a “speciation” approach demonstrated a change in the rate-determining step with increasing solution pH. This study provides not only more insight into the mechanism of dehydrogenation of FA but also offers a new principle for the design of effective homogeneous organometallic catalysts for H₂ generation from FA.},
doi = {10.1021/acscatal.5b01090},
journal = {ACS Catalysis},
number = 36,
volume = 3,
place = {United States},
year = {Thu Jul 30 00:00:00 EDT 2015},
month = {Thu Jul 30 00:00:00 EDT 2015}
}
Web of Science
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