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Metal-Thiolate Framework For Electrochemical and Photoelectrochemical Hydrogen Generations.

Hydrogen has evolved as the most clean and sustainable fuel, produced directly from naturally abundant water resources. Generation of hydrogen by electrochemical or photoelectrochemical splitting of water have been conceived as the most effective method for the hydrogen production. Herein, we first report a robust solid metal-thiolate framework (MTF-1) by hydrothermal crystallization of the reaction mixture consisting of 1,3,5-triazine-2,4,6-trithioltrisodium salt and Cu(II) under mild synthesis conditions. The material was characterized by PXRD, HRTEM, SEM, XPS, UV-visible spectroscopy. MTF-1 has been explored as efficient catalyst for electrochemical and photoelectrochemical hydrogen evolution reaction (HER) via water splitting reactions. MTF-1 showed onset potential 0.045 V RHE and η (@10 mA cm -2 ) at 0.096 V RHE . The electrochemical surface area (ECSA) of MTF-1 was found to be 509 m 2 g -1 . The photo current density at pH 5.0 was found to be 0.487 mA cm -2 at 0.6 V RHE . The feasibility of the reaction pathway is correlated from the density function theory (DFT) study, which suggested the complete downhill energetics indicating spontaneous electrochemical hydrogen generation in the acidic medium.