Operando electrochemical study demonstrates bias-induced activation of an NHC-based framework on gold for hydrogen evolution, indicating dynamic reconfiguration creates active catalytic sites.
Surface metal‐organic frameworks (SMOFs) are promising platforms for catalysis, yet their structural response to electrochemical bias is often overlooked. We report the potential‐driven activation of an N‐heterocyclic carbene (NHC)‐based SMOF on Au(111) for the hydrogen evolution reaction (HER). Operando electrochemical scanning tunneling microscopy (EC‐STM) reveals that the framework, initially “frozen” in a strongly interconnected 1D chain morphology at open circuit potential, transitions into a dynamic phase under cathodic bias. This reconfiguration involves a dynamic cycle of metal abstraction and release, generating a high density of undercoordinated sites. DFT calculations confirm that while internal bridging Au nodes are inert (ΔG H* = 0.99 eV), the potential‐induced decoupling of the chains creates terminal Au nodes and lattice vacancies with near‐thermoneutral adsorption energies of 0.05 and 0.07 eV, respectively. This study demonstrates that superior HER performance originates from the SMOF's ability to dynamically transform into a fluxional active state, providing a strategy for designing adaptive interfacial catalysts.
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Wira et al. (2026) studied this question.
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