Grafted Polymethylhydrosiloxane on Hierarchically Porous Silica Monoliths: A New Path to Monolith-Supported Palladium Nanoparticles for Continuous Flow Catalysis Applications

被引:50
作者
Pelisson, Carl-Hugo [1 ]
Nakanishi, Takahiro [1 ]
Zhu, Yang [1 ]
Morisato, Kei [2 ]
Kamei, Toshiyuki [3 ]
Maeno, Ayaka [4 ]
Kaji, Hironori [4 ]
Muroyama, Shunki [5 ]
Tafu, Masamoto [5 ]
Kanamori, Kazuyoshi [1 ]
Shimada, Toyoshi [3 ]
Nakanishi, Kazuki [1 ]
机构
[1] Kyoto Univ, Grad Sch Sci, Dept Chem, Sakyo Ku, Kyoto 6068502, Japan
[2] Kyoto Univ, GL Sci Inc, Sakyo Ku, Kyoto 6068502, Japan
[3] Nara Natl Coll Technol, Dept Chem Engn, 22 Yata Cho, Yamato Koriyama, Nara 6391080, Japan
[4] Kyoto Univ, Inst Chem Res, Kyoto 6110011, Japan
[5] Toyama Coll, Natl Inst Technol, Dept Appl Chem & Chem Engn, 13 Hongo Machi, Toyama 9398630, Japan
基金
日本科学技术振兴机构;
关键词
silica monolith; mesoporous materials; hydrosilylation; polymer; palladium nanoparticle; catalysis; selective hydrogenation; ETHENE-RICH STREAMS; MESOPOROUS SILICA; SELECTIVE HYDROGENATION; METAL NANOPARTICLES; ADSORPTION; DELIVERY; CHROMATOGRAPHY; MICROREACTORS; HYDROSILATION; ACETYLENE;
D O I
10.1021/acsami.6b12653
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Polyrnethylhydrosiloxane has been grafted on the surface of a hierarchically porous silica monolith using a facile catalytic reaction between Si-H and silanol to anchor the polymer. This easy methodology leads to the functionalization of the surface of a silica monolith, where a large amount of free Si-H bonds remain available for reducing metal ions in solution. Palladium nanoparticles of 15 nm have been synthesized homogeneously inside the mesopores of the monolith without any stabilizers, using a flow of a solution containing Pd2+. This monolith was used as column-type fixed bed catalyst for continuous flow hydrogenation of styrene and selective hydrogenation of 3-hexyn-1-ol, in each case without a significant decrease of the catalytic activity after several hours or days. Conversion, selectivity, and stereoselectivity of the alkyne hydrogenation can be tuned by flow rates of hydrogen and the substrate solution, leading to high productivity (1.57 mol g(Pd)(-1) h(-1)) of the corresponding cis-alkene.
引用
收藏
页码:406 / 412
页数:7
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