Unlocking the Ultrahigh-Current-Density Hydrogen Evolution on 2H-MoS2 via Simultaneous Structural Control across Seven Orders of Magnitude

Members of transition metal dichalcogenides, particularly molybdenum disulfide, have been recognized as promising efficient and durable earth-abundant catalysts for the hydrogen evolution reaction (HER). Despite the recent significant progress, the HER performance of MoS2 is still far from satisfactory, especially at high current densities. Here, a simultaneous multilevel structural control strategy is reported to cooperatively boost hydrogen evolution on 2H-MoS2, unlocking its potential for practical hydrogen evolution at ampere-level current densities. By confining the epitaxial growth of few-layered, curved MoS2 nanosheets within a tubular mesoporous graphitic framework, one can achieve deliberate structural control of MoS2 across seven orders of magnitude on the length scale. The resulting MoS2@C supertubes, benefiting from their unique structural features across atomic-to-microscopic scales, are characterized by abundant edge sites and sulfur vacancies, facilitated charge and mass transport, and rapid gas bubble removal. As a consequence, such MoS2@C supertubes exhibit exceptional high-current-density HER activity surpassing previously reported 2H-MoS2 catalysts and even commercial Pt/C catalysts. This work demonstrates the validity of multilevel structural engineering of 2H-MoS2 by confinement growth, opening a viable route of developing low-cost catalysts toward practical hydrogen evolution.