High-performance electrocatalysts have attracted growing interest because of their crucial roles in renewable energy technologies. In this study, the host, interlayer, and surface features of electrocatalytically-active 2D nanosheets (NSs) are systematically controlled with the synergetic combination of host−guest co-engineering and surface modification to develop a novel synthetic strategy for efficient electrocatalysts. Molecular-level control of interfacial electronic coupling and surface reactivity can be achieved by the self-assembly of MoS2/RuO2 NS mixtures with variable-sized tetraalkylammonium cations and subsequent thermal aging. The resulting optimization of the operation mechanisms of restacked MoS2/RuO2 NSs effectively improves the electrocatalyst functionality for hydrogen evolution reaction (HER). The extensive modifications of diverse structural and morphological parameters allow the elucidation of a linear correlation between electrochemical active surface area and HER overpotential. Systematic in-situ spectroscopic analyses clearly demonstrate the crucial role of enhanced Volmer−Tafel mechanism in improving the electrocatalytic activity via enhancement of proton adsorption and interfacial electron transfer.
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© 2022 Elsevier B.V.
All Science Journal Classification (ASJC) codes
- General Environmental Science
- Process Chemistry and Technology