2D layered materials, including metal-di-chalcogenides and transition metal layered double hydroxides, among others, are intensively studied because of new properties that emerge from their 2D confinement, which are attractive for advanced applications. Herein, 2D cobalt ion (Co2+) and benzimidazole (bIm) based zeolite-imidazole framework nanosheets, ZIF-9(III), are reported as exceptionally efficient electrocatalysts for the oxygen evolution reaction (OER). Specifically, liquid-phase ultrasonication is applied to exfoliate a [Co4(bIm)16] zeolite-imidazole framework (ZIF), named as ZIF-9(III) phase, into nanoscale sheets. ZIF-9(III) is selectively prepared through simple mechanical grinding of cobalt nitrate and benzimidazole in the presence of a small amount of ethanol. The resultant exfoliated nanosheets exhibit significantly higher OER activity in alkaline conditions than the corresponding bulk phases ZIF-9 and ZIF-9(III). The electrochemical and physicochemical characterization data support the assignment of the OER activity of the exfoliated nanosheet derived material to nitrogen coordinated cobalt oxyhydroxide N4CoOOH sites, following a mechanism known for Co-porphyrin and related systems. Thus, exfoliated 2D nanosheets hold promise as potential alternatives to commercial noble metal electrocatalysts for the OER.

Analytical Chemistry Center for Electrochemical Sciences Faculty of Chemistry and Biochemistry Ruhr University Bochum 44870 Bochum Germany

Center of Molecular Spectroscopy and Simulation of Solvent driven Processes Ruhr University Bochum Universitätsstr 150 44801 Bochum Germany

Chair of Inorganic and Metal Organic Chemistry Department of Chemistry and Catalysis Research Centre Technical University of Munich 85748 Garching Germany

Regional Centre of Advanced Technologies and Materials Faculty of Science Palacky University Šlechtitelu˚ 27 783 71 Olomouc Czech Republic

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