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

Abstract

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 CO_x-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.