A multicomponent assembly approach for the design of deep desulfurization heterogeneous catalysts.
A multicomponent assembly approach for the design of deep desulfurization heterogeneous catalysts.
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DOI：
10.1039/c6dt03445d
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发表时间：
2016-12
影响因子：
4
通讯作者：
Yanqi Xu;Weimin Xuan;Mengmeng Zhang;H. Miras;Yu‐Fei Song
中科院分区：
文献类型：
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作者：
Yanqi Xu;Weimin Xuan;Mengmeng Zhang;H. Miras;Yu‐Fei Song
深度脱硫是一项具有挑战性的任务，全球努力的重点是开发减少燃料油中含硫化合物的新方法。在这项工作中，我们提出了一种新的设计策略，深度脱硫非均相催化剂的发展。基于所采用的设计策略，采用剥离/接枝/组装工艺合成了一种新型的聚氧乙烯酸盐（POM）基离子液体接枝水滑石（LDHs）复合材料。采用FT-IR、XRD、TG、NMR、XPS、BET、SEM和HRTEM等手段对催化剂的结构进行了表征。该催化剂在70 °C下对DBT（二苯并噻吩）、4，6-DMDBT（4，6-二甲基二苯并噻吩）和BT（苯并噻吩）分别在25、30和40 min内表现出较高的深度脱硫活性。该催化剂易于回收，重复使用10次以上，催化活性无明显下降。这种新型多相催化剂具有优异的脱硫性能和成本效益，这是由于催化剂的设计合理，充分考虑了载体与活性中心的空间接近性、离子液体通过共价键固定在LDHs上以及催化剂的可循环性。
Deep desulfurization is a challenging task and global efforts are focused on the development of new approaches for the reduction of sulfur-containing compounds in fuel oils. In this work, we have proposed a new design strategy for the development of deep desulfurization heterogeneous catalysts. Based on the adopted design strategy, a novel composite material of polyoxometalate (POM)-based ionic liquid-grafted layered double hydroxides (LDHs) was synthesized by an exfoliation/grafting/assembly process. The structural properties of the as-prepared catalyst were characterized using FT-IR, XRD, TG, NMR, XPS, BET, SEM and HRTEM. The heterogeneous catalyst exhibited high activity in deep desulfurization of DBT (dibenzothiophene), 4,6-DMDBT (4,6-dimethyldibenzothiophene) and BT (benzothiophene) at 70 °C in 25, 30 and 40 minutes, respectively. The catalyst can be easily recovered and reused at least ten times without obvious decrease of its catalytic activity. Such excellent sulfur removal ability as well as the cost efficiency of the novel heterogeneous catalyst can be attributed to the rational design, where the spatial proximity of the substrate and the active sites, the immobilization of ionic liquid onto the LDHs via covalent bonding and the recyclability of the catalyst are carefully considered.