Publication date: 21st July 2025
Recent studies have observed that the bulky hydrophobic cations are able to promote the rate of the hydrogen evolution reaction, such as the tetrabutylammonium (TBA+). The addition of bulky hydrophobic cations provides a new perspective for optimizing electrochemical reaction which requires a molecular-level understanding on the underlying changes in the interfacial environment. We have developed a THz ATR spectroelectrochemical cell to probe molecular-level details at the gold/water interface. This innovative setup reveals the potential-dependent formation of TBA-rich film at the Au/aqueous interface. The accompanying molecular dynamics simulations quantify how the balance between electrostatic and hydrophobic solvation driving forces contributes to this observed trend. Complementary molecular simulations demonstrate that above 0.6V versus Ag/AgCl, partial TBA+ desorption induced a coadsorption of TBA+/Cl- and interfacial rehydration. Our combined experimental-theoretical approach unravel the bulky hydrophobic TBA+ cations restructure the hydrogen bond network at the metal/water interface. This allows rationalizing at the molecular level the ions-induced structural changes at the interface that tune the catalytic performances.
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