Large-scale production of H₂ through water electrolysis is limited by the lack of efficient and crust-abundant low-cost electrocatalysts. Here, MoSe₂ and N-doped carbon (NC) is successfully constructed into a double-shelled hierarchical hollow nanobox. The obtained NC@MoSe₂ is demonstrated to be an active catalyst for hydrogen evolution reaction (HER). The NC@MoSe₂ delicately combine the structural and functional advantages of two-dimensional layered transition metal dichalcogenides (TMDs) and NC, which yield the striking synergistic effect to endow them with extremely enhanced electrochemical activity to efficiently catalyze the evolution of H₂. Remarkably, the NC@MoSe₂ with the optimum thickness of MoSe₂ shell can exhibit a fairly low onset potential of 61 mV, an extremely small overpotential of 164 mV vs. RHE at 10 mA cm⁻², a greatly reduced Tafel slope of 55 mV dec⁻¹, and a higher exchange current density of 0.102 mA cm⁻². Specifically, this is mainly beneficial from the abundant exposed active edges from the edge-terminated ultrathin MoSe₂ nanosheets with small size, the overall hierarchical hollow architecture and strong electronic coupling between MoSe₂ and NC layer. Density functional theory (DFT) calculation results have well supported the experimental observations, revealing the strong synergistic effect between NC and MoSe₂, thus the increased carrier density around the Fermi level and reduced hydrogen adsorption free energy (ΔG_H*) for MoSe₂ composited with NC.

通过水电解的大规模生产H ₂受到缺乏有效且富含壳的低成本电催化剂的限制。在这里，成功地将MoSe ₂和N掺杂碳（NC）构造成双壳分层空心纳米盒。已证明所获得的NC @ MoSe ₂是用于氢释放反应（HER）的活性催化剂。NC @ MoSe ₂巧妙地结合了二维层状过渡金属二硫代双氰胺（TMDs）和NC的结构和功能优势，产生了显着的协同作用，赋予了它们极大的电化学活性，可以有效地催化H ₂的释放。值得注意的是，NC @ MoSe ₂与MOSE的最佳厚度₂外壳可表现出在10mA厘米61 mV的相当低的开始电位，一个非常小的过电压164 mV对RHE的^-2，55毫伏分解的大大减小的塔菲尔斜率^-1，和一个更高的交换电流密度为0.102 mA cm ^-2。具体而言，这主要得益于边缘端接的超薄MoSe ₂纳米片的小尺寸，整体分层的中空结构以及MoSe ₂和NC层之间的强电子耦合，从而获得了大量暴露的有源边缘。密度泛函理论（DFT）的计算结果很好地支持了实验观察，揭示了NC和MoSe ₂之间的强大协同作用，从而增加了费米能级附近的载流子密度，并降低了与NC复合的MoSe _2的氢吸附自由能（ΔGH _*）。