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In situ assembly of ultrafine Mn3O4 nanoparticles into MIL-101 for selective aerobic oxidation
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2017-08-14 00:00:00 , DOI: 10.1039/c7cy00912g
Yu Fu 1, 2, 3, 4, 5 , Yanglong Guo 1, 2, 3, 4, 5 , Yun Guo 1, 2, 3, 4, 5 , Yunsong Wang 1, 2, 3, 4, 5 , Li Wang 1, 2, 3, 4, 5 , Wangcheng Zhan 1, 2, 3, 4, 5 , Guanzhong Lu 1, 2, 3, 4, 5
Affiliation  

Nanosize metal oxides generally possess high catalytic activity, but they tend to agglomerate into larger particles during a reaction. Therefore, the preparation of nanosize metal oxides with high stability is a crucial challenge. A novel and facile approach involving impregnation followed by a double solvent method was developed to directly encapsulate ultrafine Mn3O4 nanoparticles (NPs) into the nanocages of metal–organic frameworks (MOFs). A series of MIL-101 encapsulated Mn3O4 NPs were prepared, in which the contents of Mn3O4 ranged from 3.2% to 33%. Ultrafine Mn3O4 NPs with a particle size of about 3 nm have been successfully embedded in the nanocages of MIL-101 with a uniform distribution. The MIL-101 encapsulated Mn3O4 NPs with a Mn3O4 content of 15% exhibits the highest conversion of benzyl alcohol (38.7%) and a >99% selectivity to benzaldehyde. Furthermore, after being repeatedly used 10 times, its catalytic activity is hardly changed. When the content of Mn3O4 NPs was further increased, the catalytic activity of the catalyst decreases, due to aggregated Mn3O4 particles with a large size which formed outside the MIL-101 matrix.

中文翻译:

将超细Mn 3 O 4纳米粒子原位组装到MIL-101中以进行选择性好氧氧化

纳米级金属氧化物通常具有高催化活性,但是在反应过程中它们倾向于聚集成更大的颗粒。因此,制备具有高稳定性的纳米级金属氧化物是一个关键的挑战。开发了一种新颖,简便的方法,包括浸渍和随后的双溶剂方法,以将超细Mn 3 O 4纳米颗粒(NPs)直接封装到金属有机骨架(MOFs)的纳米笼中。制备了一系列MIL-101封装的Mn 3 O 4 NP,其中Mn 3 O 4的含量为3.2%至33%。超细Mn 3 O 4已经成功地将粒径约为3 nm的NP均匀分布在MIL-101纳米笼中。Mn 3 O 4含量为15%的MIL-101封装的Mn 3 O 4 NPs表现出最高的苯甲醇转化率(38.7%)和对苯甲醛的> 99%的选择性。此外,重复使用10次后,其催化活性几乎不变。当Mn 3 O 4 NPs的含量进一步增加时,由于在MIL-101基体外部形成的大尺寸的聚集的Mn 3 O 4颗粒的聚集,催化剂的催化活性降低。
更新日期:2017-09-19
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