Hydrogen sulfide (H2S), a toxic and prevalent industrial byproduct, poses significant environmental and safety challenges, yet it also represents an underutilized source of hydrogen. The direct decomposition of H2S into hydrogen and sulfur provides a sustainable pathway for simultaneously mitigating pollution and recovering energy. However, its industrial implementation is hindered by sluggish kinetics and catalyst deactivation. Herein, a defect-rich V single-atom engineered MoS2 catalyst supported on Al2O3 (V-MoS2/Al2O3) was designed to address these challenges. Atomically dispersed V atoms possess a low coordination (3.69) environment that promotes the formation of high-density sulfur vacancies and low-valent Mo2+, thereby enhancing electron transfer and facilitating H–S bond activation. Density functional theory calculations further reveal that the formation of Mo-Svacancy-V active centers synergistically reduces the energy barriers for H2S dissociation and product (H2 and S2) desorption. The optimized catalyst achieves 72% H2S conversion with approximately ∼90% hydrogen selectivity and high-purity sulfur product at 800 °C, alongside excellent operational stability. Such high H2S conversion efficiency was achieved by the synergistic effect of the efficient catalyst developed and the fluidized-bed reactor established in this work, in which sulfur was quickly condensed and removed from the system, leading to the shift of equilibrium according to the La-Chatelier principle. This work provides fundamental insights into the cooperative mechanism of vacancy-single-atom and demonstrates a scalable atomic-level strategy for efficient hydrogen production from sulfur-rich waste streams.
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