National Engineering Research Center of Chemical Fertilizer Catalyst , Fuzhou University , Fuzhou , Fujian 350002 , P. R. China.
Inorg Chem. 2018 Aug 20;57(16):10081-10089. doi: 10.1021/acs.inorgchem.8b01232. Epub 2018 Aug 6.
Classical amino-functionalized Fe-terephthalate metal-organic framework NH-MIL-53(Fe) and its parent framework MIL-53(Fe) were prepared via simple hydrothermal methods. The catalytic performaces of these two Fe-MOFs were explored for the selective oxidation of HS. The physicochemical properties of the fresh and used Fe-MOFs catalysts were investigated by XRD, BET, SEM, FT-IR, CO-TPD, and XPS techniques. It was found that the introduction of amino groups reduces the activation energies for HS oxidation and endows this catalyst surface with moderate basic sites. As a result, the NH-MIL-53(Fe) catalyst displays high HS conversion and near 100% S selectivity in the temperature range of 130-160 °C, outperforming commercial FeO and activated carbon. Moreover, a plausible reaction route for HS selective oxidation over NH-MIL-53(Fe) is proposed. This work opens up the possibility of utilizing MOFs as efficient catalyst for desulfuration reactions.
通过简单的水热方法制备了经典的氨基官能化的 Fe-对苯二甲酸金属有机骨架 NH-MIL-53(Fe)及其母体骨架 MIL-53(Fe)。研究了这两种 Fe-MOFs 在 HS 选择性氧化中的催化性能。通过 XRD、BET、SEM、FT-IR、CO-TPD 和 XPS 技术研究了新鲜和使用过的 Fe-MOFs 催化剂的物理化学性质。结果表明，氨基的引入降低了 HS 氧化的活化能，并赋予了催化剂表面适度的碱性位。因此，NH-MIL-53(Fe)催化剂在 130-160°C 的温度范围内表现出高 HS 转化率和近 100%的 S 选择性，优于商业 FeO 和活性炭。此外，还提出了 NH-MIL-53(Fe)上 HS 选择性氧化的可能反应途径。这项工作为 MOFs 作为脱硫反应的高效催化剂开辟了可能性。
