This article describes the structural authentication of a unique triply bridged [1](ClO) and monomeric [2]ClO/[3]ClO. Electrochemical HER on a carbon cloth support demonstrated the superior performance of [1](ClO) with high TON (>10) and its long-term stability. The primary kinetic isotope effect of [1](ClO) revealed the involvement of PCET in the rate-determining step.
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