Journal
NATURE REVIEWS CHEMISTRY
Volume 2, Issue 9, Pages 244-252Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41570-018-0032-8
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Funding
- Office of Science Early Career Research Program through the US Department of Energy (DoE), Basic Energy Sciences (BES)
- US DoE BES, Chemical Sciences, Geoscience and Biosciences
- US DoE BES, Physical Biosciences
- Center for Molecular Electrocatalysis, an Energy Frontier Research Center - US DoE, Office of Science, Office of BES
- Indian Institute of Technology (IIT) Gandhinagar
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The most energy-efficient electrocatalysts mediate forward and reverse reactions at high rates with minimal overpotential requirements. Such electrocatalytic reversibility is commonly observed for redox enzymes and is an attribute that we have sought to bestow on synthetic molecules to realize highly active and robust catalysts for applications in renewable energy. The recent development of the first synthetic molecular catalysts that reversibly mediate H-2 (sic) 2H(+) + 2e(-) exploits an enzyme-inspired outer coordination sphere that works in concert with both first and second coordination spheres. In this Perspective, we discuss a series of molecular Ni catalysts for H-2 production and oxidation that exhibit electrochemical reversibility. Study of these catalysts allows us to identify important first, second and outer coordination sphere features necessary for efficient conversions of H-2 and provides direction for the rational design of electrocatalysts that operate on other small molecules.
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