Keggin-POM@rht-MOF-1 composite as heterogeneous catalysts towards ultra-deep oxidative fuel desulfurization
Keggin-POM@rht-MOF-1 composite as heterogeneous catalysts towards ultra-deep oxidative fuel desulfurization
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DOI：
10.1016/j.fuel.2020.117834
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发表时间：
2020-08
期刊：
影响因子：
7.4
通讯作者：
Pengpeng Wei;Yang Yang-Yang;Weizuo Li;Guangming Li
中科院分区：
文献类型：
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作者：
Pengpeng Wei;Yang Yang-Yang;Weizuo Li;Guangming Li
POM@MOF复合材料因其惊人的催化性能、可靠的稳定性和可回收性而备受关注；然而，合成预期的POM@MOF复合材料和催化有机反应仍然是巨大的挑战。在此，通过使用rht-MOF-1的大内腔窗口封装客体分子，分离出一系列三个Keggin-POM@rht-MOF-1（POM=H3+nPMo12-nVnO40，n=1，（Mo11V1）；n=2，（Mo10V2）；n=3，（Mo9V3））凯金-POM。 X射线晶体分析表明Keggin-POM@rht-MOF-1复合材料具有高负载效率和化学稳定性。合成的Keggin-POM@rht-MOF-1复合材料用作模型柴油和真实柴油脱硫反应的催化剂后，Mo9V3和Mo9V3的脱硫转化率分别高达96%和90%。其衍生物兼具了主体（rht-MOF-1）和客体Keggin-POM的优点。尺寸匹配的rht-MOF-1阻止了Keggin-POM的浸出，而Keggin-POM保留了二苯并噻吩（DBT）、1-苯并噻吩（BT）和4,6-二甲基二苯并噻吩（4,6-DMDBT）的可达性以催化氧化反应。
POM@MOF composites have aroused much concern regarding their amazing catalytic performance, reliable stability and recyclability; however, it remains great challenge on synthesizing expected POM@MOF composites and catalyzing organic reactions. Herein, a series of three Keggin-POM@rht-MOF-1 (POM = H3+nPMo12-nVnO40, n = 1, (Mo11V1); n = 2, (Mo10V2); n = 3, (Mo9V3)), have been isolated by using a large internal cavity window ofrht-MOF-1 to encapsulate the guest molecules of Keggin-POM. X-ray crystallographic analysis reveals that Keggin-POM@rht-MOF-1 composites are of high load efficiency and chemical stability. Upon employed as catalysts on the desulfurization reaction of model diesels and real diesels, the as-synthesized Keggin-POM@rht-MOF-1 composites exhibit high percent conversion of desulfurization up to 96% byMo9V3and 90% byMo9V3, respectively. Its derivatives from both the advantages of the host ofrht-MOF-1) and the Keggin-POM guest. The size-matchedrht-MOF-1 prevented the leaching of Keggin-POM, while the Keggin-POM retain the reachability of dibenzothiophene (DBT), 1-benzothiophene (BT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT) for the catalyzing the oxidation reactions.