Reversing the Tradeoff between Rate and Overpotential in Molecular Electrocatalysts for H2 Production
Abstract
A long-standing challenge in molecular electrocatalysis is to design catalysts that break away from the tradeoff between rate and overpotential arising from electronic scaling relationships. Here we report an inversion of the rate-overpotential correlation through system-level design of new [Ni(PR2NR'2)2]2+ electrocatalysts for the production of H2. The overpotential is lowered by an electron-withdrawing ligand, while the turnover frequency is increased by controlling the catalyst structural dynamics, using both ligand design and solvent viscosity. Here, the cumulative effect of controlling each of these system components is an electrocatalyst with a turnover frequency of 70,000 s–1 and an overpotential of 230 mV, corresponding to a 100-fold rate enhancement and a 170 mV reduction in overpotential compared to the parent nickel catalyst. The success of this system-level approach originates from the detailed mechanistic understanding of these catalysts, which enabled modifications of the catalyst and solvent to disfavor non-productive pathways.
- Authors:
-
[1];
[1]
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States); State Univ. of New York, Fredonia, NY (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Molecular Electrocatalysis (CME); Battelle Memorial Institute, Columbus, OH (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1566354
- Alternate Identifier(s):
- OSTI ID: 1842948
- Report Number(s):
- PNNL-SA-130125
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 4; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous); catalysis (heterogeneous); solar (fuels); bio-inspired; energy storage (including batteries and capacitors); hydrogen and fuel cells; charge transport; materials and chemistry by design; synthesis (novel materials); electrocatalysis; hydrogen; scaling relation; overpotential; nickel; proton relay; viscosity; reaction mechanism; amines; electrocatalysts; catalystsl solvents
Citation Formats
Klug, Christina M., Cardenas, Allan Jay P., Bullock, R. Morris, O’Hagan, Molly, and Wiedner, Eric S. Reversing the Tradeoff between Rate and Overpotential in Molecular Electrocatalysts for H2 Production. United States: N. p., 2018.
Web. doi:10.1021/acscatal.7b04379.
Klug, Christina M., Cardenas, Allan Jay P., Bullock, R. Morris, O’Hagan, Molly, & Wiedner, Eric S. Reversing the Tradeoff between Rate and Overpotential in Molecular Electrocatalysts for H2 Production. United States. https://doi.org/10.1021/acscatal.7b04379
Klug, Christina M., Cardenas, Allan Jay P., Bullock, R. Morris, O’Hagan, Molly, and Wiedner, Eric S. Wed .
"Reversing the Tradeoff between Rate and Overpotential in Molecular Electrocatalysts for H2 Production". United States. https://doi.org/10.1021/acscatal.7b04379. https://www.osti.gov/servlets/purl/1566354.
@article{osti_1566354,
title = {Reversing the Tradeoff between Rate and Overpotential in Molecular Electrocatalysts for H2 Production},
author = {Klug, Christina M. and Cardenas, Allan Jay P. and Bullock, R. Morris and O’Hagan, Molly and Wiedner, Eric S.},
abstractNote = {A long-standing challenge in molecular electrocatalysis is to design catalysts that break away from the tradeoff between rate and overpotential arising from electronic scaling relationships. Here we report an inversion of the rate-overpotential correlation through system-level design of new [Ni(PR2NR'2)2]2+ electrocatalysts for the production of H2. The overpotential is lowered by an electron-withdrawing ligand, while the turnover frequency is increased by controlling the catalyst structural dynamics, using both ligand design and solvent viscosity. Here, the cumulative effect of controlling each of these system components is an electrocatalyst with a turnover frequency of 70,000 s–1 and an overpotential of 230 mV, corresponding to a 100-fold rate enhancement and a 170 mV reduction in overpotential compared to the parent nickel catalyst. The success of this system-level approach originates from the detailed mechanistic understanding of these catalysts, which enabled modifications of the catalyst and solvent to disfavor non-productive pathways.},
doi = {10.1021/acscatal.7b04379},
journal = {ACS Catalysis},
number = 4,
volume = 8,
place = {United States},
year = {Wed Mar 07 00:00:00 EST 2018},
month = {Wed Mar 07 00:00:00 EST 2018}
}
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