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Synergistic effects of MOF-76 on layered double hydroxides with superior activity for extractive catalytic oxidative desulfurization
New Journal of Chemistry ( IF 3.3 ) Pub Date : 2020-03-17 , DOI: 10.1039/d0nj00612b
Siqi Liu 1, 2, 3, 4, 5 , Xiaonan Li 1, 2, 3, 4, 5 , Hong Zhang 1, 2, 3, 4, 5
Affiliation  

The combination of metal–organic frameworks (MOFs) with layered double hydroxides (LDHs) has been greatly limited by the agglomeration of pure MOFs and the height of the LDH gallery, so there are few reports on the combination of MOFs and LDHs. In this work, for the first time, the combination of MOF-76 with a layered double hydroxide (MOF-76@LDH) was used for desulfurization under room temperature and pressure conditions without the necessity of protecting with nitrogen. The structure of the heterogeneous catalyst was characterized using FT-IR, XRD, TG, BET, SEM, EDX, XPS, fluorescence and ICP-AES. The as-prepared catalyst exhibited superior activity in deep desulfurization of DBT (dibenzothiophene), BT (benzothiophene) and 4,6-DMDBT (4,6-dimethyldibenzothiophene). The above sulfides could be completely converted into their corresponding sulfones and sulfoxides at 60 °C in 25, 40 and 55 minutes, respectively. 49 wt% MOF-76@LDH exhibited a high desulfurization capacity (100%), much higher than that of LDH (16.3%), MOF-76 (48%) and MOF-76 + LDH (50.3%). Because MOF-76@LDH has a special one-dimensional channel on the surface of the material, it can efficiently promote the degradation of H2O2 into hydroxyl radicals (˙OH) and further improve the desulfurization effect. The catalyst is easy to recycle and can be reused at least 5 times, and the catalytic effect is not significantly reduced. This provides a completely new route for the synthesis of MOF–LDH advanced functional materials.

中文翻译:

MOF-76对层状双氢氧化物的协同作用,对萃取催化氧化脱硫具有优异的活性

金属有机骨架(MOF)与层状双氢氧化物(LDH)的结合受到纯MOF的团聚和LDH通道高度的限制,因此,关于MOF和LDH结合的报道很少。在这项工作中,MOF-76与层状双氢氧化物(MOF-76 @ LDH)的组合首次在室温和压力条件下用于脱硫,而无需使用氮气进行保护。使用FT-IR,XRD,TG,BET,SEM,EDX,XPS,荧光和ICP-AES对非均相催化剂的结构进行了表征。所制备的催化剂在DBT(二苯并噻吩),BT(苯并噻吩)和4,6-DMDBT(4,6-二甲基二苯并噻吩)的深度脱硫中表现出优异的活性。上述硫化物可以分别在60°C,25、40和55分钟内完全转化为相应的砜和亚砜。49 wt%的MOF-76 @ LDH具有高脱硫能力(100%),远高于LDH(16.3%),MOF-76(48%)和MOF-76 + LDH(50.3%)。由于MOF-76 @ LDH在材料表面上具有特殊的一维通道,因此可以有效地促进H的降解2 O 2转变为羟基自由基(= OH),进一步提高了脱硫效果。该催化剂易于回收并且可以重复使用至少5次,并且催化效果没有显着降低。这为合成MOF-LDH高级功能材料提供了一条全新的途径。
更新日期:2020-03-17
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