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Hydrogen sulfide is characterized with strong toxicity and corrosivity, so it is important to efficiently minimize its pollution. In this laboratory experiment a series of HPAs@UiO-66 were prepared by one-step hydrothermal method with molybdenum-based heteropoly acid (HPAs) as active centers and UiO-66 as a carrier, and a multi-acid-based solid phase desulfurization system with various active centers was set up. The effects of Keggin and Dawson structures, the central atoms (P and Si), and the substitutional atoms (V and W) of HPAs on desulfurization performance were studied, and their physico-chemical properties were analyzed by BET, FT-IR, XRD, SEM, and TEM. As a result, it was showed that PMo12@UiO-66 had excellent desulfurization activity, its H2S removal ability was maximized at 100 °C with a absorbing capacity being able to reach 17.18 mg/g, and it was found the presence of water in the mixed gas can promote PMo12@UiO-66 to remove H2S. In comparison with PMo12 and UiO-66, PMo12@UiO-66 was far better in desulfurization, its H2S absorbing capacity was 7.5 and 14.2 times PMo12 and UiO-66, respectively, demonstrating the synergistic desulfurization effect of PMo12 and UiO-66. Analysis by use of XPS (X-ray photo-electron spectroscopy) showed that the redox reaction took place between PMo12 and H2S, during which H2S was converted into elemental sulfur due to the oxidizing action of PMo12. In conclusion, this study proved that the introduction of PM012 had exhibited the most remarkable effect on enforcing the desulfurization performance of UiO-66, which could provide a reference for exploiting more novel HPA-based solid phase desulfurization agents. [ABSTRACT FROM AUTHOR]