Aromaticity Driven Electrocatalytic Water Oxidation by a Phosphorus-Nitrogen PN3-Pincer Cobalt Complex
KAUST DepartmentKAUST Catalysis Center and Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia
KAUST Catalysis Center (KCC)
Chemical Science Program
Physical Sciences and Engineering (PSE) Division
Permanent link to this recordhttp://hdl.handle.net/10754/656868
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AbstractWater oxidation is the primary step in both natural and artificial photosynthesis to convert solar energy in into chemical fuels. Herein, we report the first cobalt-based pincer catalyst for electrolytic water oxidation at neutral pH with high efficiency under electrochemical conditions. Most importantly, ligand (pseudo)aromaticity is identified to play an important role in the electrocatalysis. A significant potential jump (~300 mV) was achieved towards a lower positive value when the aromatized cobalt complex was transformed to a (pseudo)dearomatized cobalt species. This complex catalyzes the water oxidation in its high valent oxidation state at a much lower overpotential (~ 340 mV vs. NHE) based on the onset potential (0.5 mA/cm<sup>2</sup>) of catalysis at pH 10.5, outperforming all the other literature systems. These observations may provide a new strategy for the design of earth-abundant transition metal-based water oxidation catalysts.
CitationDas, P. K., Bhunia, S., Chakraborty, P., Rana, A., Dey, A., & Huang, K.-W. (2019). Aromaticity Driven Electrocatalytic Water Oxidation by a Phosphorus-Nitrogen PN3-Pincer Cobalt Complex. doi:10.26434/chemrxiv.9729878
SponsorsThis work is supported by King Abdullah University of Science and Technology and Department of Science and Technology grant DST/TMD/HFC/2k18/90 by government of India.