Defect-Rich Molybdenum Disulfide for Improved Hydrogen Production via H₂S Reforming with CH₄

H2S reforming with CH4 (H2SMR) provides a viable approach for the elimination of hazardous H2S and the direct utilization of sour natural gas, efficiently producing COx-free H2 while simultaneously yielding high-value-added sulfur chemicals. Herein, MoS2 catalysts enriched with edge sites and sulfur vacancy defects were fabricated via a cost-effective one-step solvothermal synthesis method and examined for the H2SMR reaction. MoS2 synthesized using ethylene glycol (EG) solvent (MoS2-EG) presented oxygen doping and featured fewer layers and a larger interlayer spacing, thus possessing abundant active edge sites and sulfur vacancy defects. Consequently, MoS2-EG demonstrated exceptional hydrogen production efficiency and stability, achieving a hydrogen yield of 8.5 mmol/(g min) at 900 °C and a H2S/CH4 molar ratio of 3. The abundant defects and edge sites in MoS2-EG contributed to the facile H2S activation to preferentially form reactive sulfur species for C–H bond activation, which is responsible for the superior H2SMR activity. This study significantly advances the development of high-efficiency, scalable catalysts for H2SMR, presenting a transformative approach to utilizing sour natural gas as a resource while addressing environmental challenges.