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Ga III chloride tetrakis(pentafluorophenyl)porphyrin ( 1 ) was synthesized and shown to be a highly active and stable post-transition metal-based electrocatalyst for the hydrogen evolution reaction (HER). Electrochemical and spectroscopic studies indicate that both the first and second reduction events of 1 are ligand-centered. The 2e-reduced form 1  2- reacts with a proton to give Ga III -H species ( 1 -H), which undergoes protonolysis with Brønsted acids to produce H 2 . The identification of key intermediates 1  - , 1  2- , and 1 -H leads to a catalytic cycle, which is valuable for the fundamental understanding of the HER. This study presents a rare but highly active HER electrocatalyst with unusual features, including ligand-centered electron transfer and formation of post-transition metal hydride.

Electrocatalytic hydrogen evolution with gallium hydride and ligand-centered reduction