Synthesis of framework-substituted Fe-HMS and its catalytic performance for phenol hydroxylation

Synthesis of framework-substituted Fe-HMS and its catalytic performance for phenol hydroxylation
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DOI:
10.1088/0957-4484/17/4/026
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发表时间:
2006-02
期刊:
影响因子:
3.5
通讯作者:
Hong Liu;G. Lu;Yanglong Guo;Yun Guo;Junsong Wang
Hong Liu;G. Lu;Yanglong Guo;Yun Guo;Junsong Wang
中科院分区:
材料科学3区
文献类型:
--
作者:
Hong Liu;G. Lu;Yanglong Guo;Yun Guo;Junsong Wang

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以十二胺为模板剂,在室温下成功合成了铁掺杂介孔氧化硅材料Fe-HMS,并通过XRD、SEM、FT-IR、UV-vis、ESR和N2吸附等手段对其进行了表征。在固定床反应器中考察了该催化剂对苯酚过氧化氢羟基化反应的催化性能。结果表明,Fe 3+离子已成功地嵌入HMS的骨架中,Fe-HMS具有均匀的介孔结构,孔径约为2.7 nm。焙烧后,大部分Fe ~(3+)离子仍保留在四面体配位骨架中,只有一小部分Fe物种迁移到骨架外。Fe-HMS对苯酚羟基化反应具有很高的催化活性和选择性。在Fe-HMS催化剂上苯酚羟基化反应的产物分布与微孔TS-1分子筛上的不同。溶剂对Fe-HMS的催化活性有很大影响,水是最佳溶剂。
The iron-incorporated mesoporous silica material Fe-HMS was successfully synthesized at ambient temperature by using dodecylamine as the template agent, and it was characterized by XRD, SEM, FT–IR, UV–vis, ESR and N2 adsorption measurements. Its catalytic performance was studied for phenol hydroxylation with H2O2 in a fixed-bed reactor. The results show that Fe3+ ions have been successfully incorporated into the framework of HMS, and Fe-HMS has a uniform mesoporous structure with about 2.7 nm pore diameter. After Fe-HMS is calcined, most of the Fe3+ ions remain in the tetrahedral coordinated framework, and only a small part of Fe species migrate to the extraframework. Fe-HMS has high catalytic activity and very high selectivity to dihydroxybenzene for the hydroxylation of phenol. Over the Fe-HMS catalyst, the product distribution of phenol hydroxylation is different from that over the microporous TS-1 zeolite. The solvents have great influence on the catalytic activity of Fe-HMS, and water is the best solvent.