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Photochemical H2 Evolution from Bis(diphosphine)nickel Hydrides Enables Low-Overpotential Electrocatalysis
Bethany M Stratakes1, Kaylee A Wells2, Daniel A Kurtz1
1Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599-3290, United States.
Journal of the American Chemical Society
|December 8, 2021
Summary
Researchers developed nickel photoelectrocatalysts for efficient hydrogen (H₂) evolution using visible light. This breakthrough enables solar fuel generation without high overpotentials or semiconductor materials.
Area of Science:
- Photochemistry
- Catalysis
- Materials Science
Background:
- First-row transition metal complexes are sought for solar fuel applications.
- Efficient light-harvesting and bond-forming catalysts are crucial for solar fuel generation.
Purpose of the Study:
- To report novel nickel photoelectrocatalysts for hydrogen evolution.
- To elucidate the mechanism of visible-light-driven H₂ evolution.
Main Methods:
- Utilized bis(diphosphine)nickel hydride complexes.
- Employed time-resolved spectroscopy and quantum yield measurements.
- Conducted thermodynamic analyses.
Main Results:
- Demonstrated visible-light-driven H₂ evolution using nickel complexes.
- Proposed a mechanism involving Ni-H bond homolysis from a singlet excited state.
- Achieved over 500 mV improvement in electrochemical overpotential under illumination, enabling H₂ evolution at 0 mV overpotential.
Conclusions:
- Nickel complexes can function as efficient photoelectrocatalysts for H₂ evolution.
- Understanding first-row transition metal hydride photochemistry is key for catalyst design.
- This system offers a pathway to solar fuel generation without sacrificial agents or semiconductors.
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