Fe/Zr-SBA-15的制备及其催化氧化脱硫性能

Preparation of Fe/Zr-SBA-15 catalyst and its oxidative desulfurization performance

  • 摘要: 为进一步提高氧化脱硫效果,采用直接水热法合成了不同Fe/Zr物质的量比改性的SBA-15分子筛(Fe/Zr-SBA-15),采用XRD、N2吸附-脱附、TEM和UV-vis等对其进行了表征。Fe/Zr-SBA-15中Zr取代Si进入了分子筛骨架,大部分Fe物种分散良好,存在少量的聚集态铁的氧化物。以Fe/Zr-SBA-15-1.0为催化剂、H2O2为氧化剂、乙腈为萃取剂,分别考察了反应温度、O/S物质的量比和催化剂用量对模拟油中二苯并噻吩(DBT)的氧化效果。在反应温度50 ℃,O/S物质的量比为4,催化剂用量6 g/L的条件下,DBT的脱除率达到97.1%,这是由于催化剂中的Fe3 + 提供氧化活性中心和Zr4 + 提供的吸附中心的双重作用,且催化剂回收利用四次后,DBT的脱除率仍可达到91.3%。

     

    Abstract: To improve the oxidative desulfurization performance, the modified SBA-15 (Fe/Zr-SBA-15) with different Fe/Zr molar ratios were synthesized by direct hydrothermal method. The samples were characterized by XRD, N2 adsorption and desorption, TEM and UV-vis. Zr was incorporated into the framework of SBA-15. Apart from little aggregated iron oxides, most of the Fe species were well dispersed in Fe/Zr-SBA-15. The influence of the reaction temperature, amount of oxidant and dosage of catalyst on the conversion of DBT were investigated using Fe/Zr-SBA-15-1.0 as catalyst, H2O2 as oxidant and acetonitrile as extractant. The removal rate of DBT reached 97.1% under the conditions of reaction temperature 50 ℃, O/S molar ratio of 4 and catalyst dosage of 6 g/L. The synergistic effect of Fe and Zr played important role, with Fe3 + acting as the oxidation activity center and Zr4 + as the center of adsorption. In addition, the removal rate of DBT could still reach 91.3% after 4 cycles and Fe/Zr-SBA-15 showed good stability.

     

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