CNTs Bridged Basal-Plane-Active 2H-MoS₂ Nanosheets for Efficient Robust Electrocatalysis

2D 2H-phase MoS₂ is promising for electrocatalytic applications because of its stable phase, rich edge sites, and large surface area. However, the pristine low-conductive 2H-MoS₂ suffers from limited electron transfer and surface activity, which become worse after their highly likely aggregation/stacking and self-curling during applications. In this work, these issues are overcome by conformally attaching the intercalation-detonation-exfoliated, surface S-vacancy-rich 2H-MoS₂ onto robust conductive carbon nanotubes (CNTs), which electrically bridge bulk electrode and local MoS₂ catalysts. The optimized MoS₂/CNTs nanojunctions exhibit outstanding stable electroactivity (close to commercial Pt/C): a polarization overpotential of 79 mV at the current density of 10 mA cm⁻² and the Tafel slope of 33.5 mV dec⁻¹. Theoretical calculations unveil the metalized interfacial electronic structure of MoS₂/CNTs nanojunctions, enhancing defective-MoS₂ surface activity and local conductivity. This work provides guidance on rational design for advanced multifaceted 2D catalysts combined with robust bridging conductors to accelerate energy technology development.