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

Abstract

Abstract2D 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.