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MoSx-on-Nitrogen Doped Graphene for High-Efficiency Hydrogen Evolution Reaction: Unraveling the Mechanisms of Unique Interfacial Bonding for Efficient Charge Transport and Stability.

Functional nanostructures with abundant exposed active sites and facile charge transport through conductive scaffolds to active sites are pivotal for developing an advanced and efficient electrocatalyst for water splitting. In the present study, by coating ~ 3 nm MoSx on nitrogen-doped graphene (NG) pre-engrafted on a flexible carbon cloth (MNG) as a model system, an extremely low Tafel slope of 39.6 mV dec-1 with cyclic stability up to 5000 cycles is obtained. The specific fraction of N on NG framework is also varied by X-ray photoelectron spectroscopy and X-ray absorption near edge spectroscopy with synchrotron radiation light sources, and it is found that the MoSx particles are selectively positioned on the specific graphitic N sites, forming the unique Mo-N-C bonding state. This Mo-N-C bonding is founded to facilitate highly effective charge transfer directly to the active sulfur sites on the edges of MoSx, lead to a highly improved hydrogen evolution reaction (HER) with excellent stability (95% retention @ 5000 cycles). The functional anchoring of MoSx by such bonding preventing particles aggregation, which plays a significant role in maintaining the stability and activity of the catalyst. Furthermore, it has been revealed that MNG samples with adequately high amounts of both pyridinic and graphitic N result in best HER performance. This work helps for understanding the mechanisms and bonding interactions within the various catalyst and the scaffold electrode.