The lack of highly efficient, inexpensive catalysts severely hinders large-scale application of electrochemical hydrogen evolution reaction (HER) for producing hydrogen. MoS₂ as a low-cost candidate suffers from low catalytic performance. Herein, taking advantage of its tri-layer structure, we report a MoS₂ nanofoam catalyst co-confining selenium in surface and cobalt in inner layer, exhibiting an ultra-high large-current-density HER activity surpassing all previously reported heteroatom-doped MoS₂. At a large current density of 1000 mA cm⁻², a much lower overpotential of 382 mV than that of 671 mV over commercial Pt/C catalyst is achieved and stably maintained for 360 hours without decay. First-principles calculations demonstrate that inner layer-confined cobalt atoms stimulate neighbouring sulfur atoms while surface-confined selenium atoms stabilize the structure, which cooperatively enable the massive generation of both in-plane and edge active sites with optimized hydrogen adsorption activity. This strategy provides a viable route for developing MoS₂-based catalysts for industrial HER applications.

缺乏高效、廉价的催化剂严重阻碍了电化学析氢反应（HER）在制氢中的大规模应用。MoS ₂作为低成本的候选者，催化性能低。在此，利用其三层结构，我们报道了一种将硒共限制在内层的MoS ₂纳米泡沫催化剂，表现出超高大电流密度的HER活性，超过了之前报道的所有杂原子掺杂的MoS ₂ . 在 1000 mA cm ^{-2的大电流密度下}，在商业 Pt/C 催化剂上实现了比 671 mV 低得多的 382 mV 过电位，并稳定保持 360 小时而不衰减。第一性原理计算表明，内层限制的钴原子刺激相邻的硫原子，而表面限制的硒原子稳定了结构，从而协同产生大量具有优化氢吸附活性的面内和边缘活性位点。该策略为开发用于工业 HER 应用的 MoS ₂基催化剂提供了一条可行的途径。