Kinetic-Oriented Construction of MoS₂ Synergistic Interface to Boost pH-Universal Hydrogen Evolution

As a prerequisite for a sustainable energy economy in the future, designing earth-abundant MoS₂ catalysts with a comparable hydrogen evolution catalytic performance in both acidic and alkaline environments is still an urgent challenge. Decreasing the energy barriers could enhance the catalysts' activity but is not often a strategy for doing so. Here, the first kinetic-oriented design of the MoS₂-based heterostructure is presented for pH-universal hydrogen evolution catalysis by optimizing the electronic structure based on the simultaneous modulation of the 3d-band-offsets of Ni, Co, and Mo near the interface. Benefiting from this desirable electronic structure, the obtained MoS₂/CoNi₂S₄ catalyst achieves an ultralow overpotential of 78 and 81 mV at 10 mA cm⁻², and turnover frequency as high as 2.7 and 1.7 s⁻¹ at the overpotential of 200 mV in alkaline and acidic media, respectively. The MoS₂/CoNi₂S₄ catalyst represents one of the best hydrogen evolution reaction performing ones among MoS₂-based catalysts reported to date in both alkaline and acidic environments, and equally important is the remarkable long-term stability with negligible activity loss after maintaining at 10 mA cm⁻² for 48 h in both acid and base. This work highlights the potential to deeply understand and rationally design highly efficient pH-universal electrocatalysts for future energy storage and delivery.