Title : Aromaticity-Driven electrocatalytic water splitting by pincer-type cobalt-based complex
Abstract:
Water electrolysis is a promising method toward hydrogen production, requiring only water and electricity. Splitting water into oxygen and hydrogen using inexpensive and bi-functional electrocatalysts and renewable electricity is crucial in addressing contemporary energy and environmental issues. A cobalt-pincer complex, when oxidized in air, is found to be soluble and stable in water and forms an electron-deficient complex, providing a greater thermodynamic driving force for water oxidation. The electronic property of the complex makes it one of the best catalysts for electrochemical water splitting at room temperature in neutral aqueous solutions, outperforming many of the previously reported electrocatalysts. In addition, the study identified the crucial role of ligand (pseudo)aromaticity in electrocatalysis. It showcased that the dearomatized species showed better activity for the water oxidation reaction (OER), while aromatized species exhibited better activity for the hydrogen evolution reaction (HER) at a significantly lower overall overpotential (~ 0.48 V), outperforming other Co-based molecular catalysts reported. This molecular system was robust under electrochemical conditions, showing negligible decomposition over hours of operation.