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A bioinspired cobalt catalyst based on a tripodal imidazole/pyridine platform capable of water reduction and

Krista M Kulesa¹, Diego S Padilha², Bishnu Thapa¹

¹Department of Chemistry, Wayne State University, 5101 Cass Avenue, Detroit, MI 48202, USA.

Journal of Inorganic Biochemistry

|February 25, 2023

Abstract:

The prototypical drug carrier [Co^II(L¹)Cl]PF₆ (1), where L¹ is a tripodal amine bound to pyridine and methyl-imidazoles, had its electrocatalytic water splitting activity studied under different pH conditions. This species contains a high-spin 3d⁷ Co^II metal center, and is capable of generating both H₂ from water reduction and O₂ from water oxidation_. Turnover numbers reach 390 after 3 h for water reduction. Initial water oxidation activity is molecular, with TONs of 71 at pH 7 and 103 at pH 11.5. The results reveal that species 1 can undergo several redox transformations, including reduction to the 3d⁸ Co^I species that precedes a ^LS3d⁶ hydride for water reduction, as well as nominal Co^IVO and Co^III-OOH species required for water oxidation. Post-catalytic analyses confirm the molecular nature of reduction and support initial molecular activity for oxidation.

Keywords:

Bioinorganic Cobalt complex Drug carrier repurposed Electrocatalysis Water oxidation Water reduction

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