AbstractFabrication of two‐dimensional electrocatalysts with low cost and high efficiency is of great significance for electrochemical hydrogen evolution reaction (HER). Molybdenum disulfide (MoS2) is one of the most promising alternatives to Pt‐based HER catalysts, however its electrocatalytic performance is greatly limited by insufficient active edge sites and poor conductivity. Herein, ZIF‐8‐derived nitrogen‐doped carbon sheet (NCS) is utilized as the support, and the heterostructure of NCS@MoS2 is assembled by a facile hydrothermal reaction between MoS2 precursor and NCS. This is the first example of NCS‐supported MoS2 structures for HER application. The results show that defect‐rich MoS2 ultrathin nanosheets are uniformly and vertically aligned on NCS, and the dispersion degree of MoS2 can be well controlled by adjusting the surface modification of NCS. As expected, the optimized catalyst possesses a superior catalytic performance to pristine MoS2 evidenced by a low overpotential (250 mV) to afford 10 mA cm−2, and a small Tafel slope (74 mV dec−1) with good stability in acidic media. The intriguing HER activity is attributed to the synergistic effect of abundantly exposed active sites and high conductivity.
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