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

Abstract As a prerequisite for a sustainable energy economy in the future, designing earth‐abundant MoS 2 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 MoS 2 ‐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 MoS 2 /CoNi 2 S 4 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 MoS 2 /CoNi 2 S 4 catalyst represents one of the best hydrogen evolution reaction performing ones among MoS 2 ‐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.