597-52-4Relevant articles and documents
Heterogeneous nickel catalyst for selective hydration of silanes to silanols
Shimizu, Ken-Ichi,Shimura, Katsuya,Imaiida, Naomichi,Satsuma, Atsushi
, p. 50 - 54 (2012)
Selective catalytic hydration of silanes to silanols is studied by Ni metal nanoparticles (NPs) on activated carbon (Ni/C) prepared by in situ H 2-reduction of NiO-loaded activated carbon (NiO/C). The catalytic activity of Ni/C increases with decrease in the average Ni particle size. Ni/C with the smallest size (7.6 nm) exhibits a high selectivity for silanols, high turnover number (TON) of 9300, and excellent reusability. Studies on the structure-activity relationship show that metallic Ni species on the surface of small Ni metal particles are catalytically active species. Based on mechanistic studies, a catalytic cycle involving the activation of Et3SiH as the rate limiting step is proposed.
Hydrosilane-assisted formation of metal nanoparticles on graphene oxide
Saito, Akinori,Kinoshita, Hiroshi,Shimizu, Ken-Ichi,Nishina, Yuta
, p. 67 - 73 (2016)
Metal nanoparticles were formed on graphene oxide by a deposition process with hydrosilane, giving thin layer metalgraphene oxide (metal/GO) composites. The particle size and catalytic activity could be controlled by varying the hydrosilane amount. Hydrosilane prevented the aggregation of GO layers by surface functionalization via silane coupling reaction. The metal/GO composites were evaluated as catalysts in hydrosilane oxidation.
Generation of 1Δg O2 from Triethylsilane and Ozone
Corey, E. J.,Mehrotra, Mukund M.,Khan, Ahsan U.
, p. 2472 - 2473 (1986)
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Cobalt single atoms anchored on nitrogen-doped porous carbon as an efficient catalyst for oxidation of silanes
Yang, Fan,Liu, Zhihui,Liu, Xiaodong,Feng, Andong,Zhang, Bing,Yang, Wang,Li, Yongfeng
, p. 1026 - 1035 (2021/02/09)
The oxidation reactions of organic compounds are important transformations for the fine and bulk chemical industry. However, they usually involve the use of noble metal catalysts and suffer from toxic or environmental issues. Here, an efficient, environmentally friendly, and atomically dispersed Co catalyst (Co-N-C) was preparedviaa simple, porous MgO template and etching method using 1,10-phenanthroline as C and N sources, and CoCl2·6H2O as the metal source. The obtained Co-N-C catalyst exhibits excellent catalytic performance for the oxidation of silanes with 97% isolated yield of organosilanol under mild conditions (room temperature, H2O as an oxidant, 1.8 h), and good stability with 95% isolated yield after nine consecutive reactions. The turnover frequency (TOF) is as high as 381 h?1, exceeding those of most non-noble metal catalysts and some noble metal catalysts. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), extended X-ray absorption fine structure (EXAFS), and wavelet transform (WT) spectroscopy corroborate the existence of atomically dispersed Co. The coordination numbers of Co affected by the pyrolysis temperature in Co-N-C-700, Co-N-C-800, and Co-N-C-900 are 4.1, 3.6, and 2.2, respectively. Owing to a higher Co-N3content, Co-N-C-800 shows more outstanding catalytic performance than Co-N-C-700 and Co-N-C-800. Moreover, density functional theory (DFT) calculations reveal that the Co-N3structure exhibits more activity compared with Co-N4and Co-N2, which is because the Co atom in Co-N3was bound with both H atom and Si atom, and it induced the longest Si-H bond.
Integration of Pd nanoparticles with engineered pore walls in MOFs for enhanced catalysis
Li, Luyan,Li, Zhixin,Yang, Weijie,Huang, Yamin,Huang, Gang,Guan, Qiaoqiao,Dong, Yemin,Lu, Junling,Yu, Shu-Hong,Jiang, Hai-Long
, p. 686 - 698 (2021/02/27)
Achieving free-access metal sites with the ability to regulate interactions with substrates is highly desired yet remains a grand challenge in catalysis. Herein, naked Pd nanoparticles were encapsulated inside a metal-organic framework (MOF), giving Pd@MIL-101-NH2. Its activity and selectivity toward de/hydrogenation reactions can be greatly promoted via the MOF pore wall engineering to regulate Pd surrounding microenvironment and substrate adsorption behavior. Creating free-access active sites and regulating their interaction with substrates are crucial for efficient catalysis, yet remain a grand challenge. Herein, naked Pd nanoparticles (NPs) have been encapsulated in a metal-organic framework (MOF), MIL-101-NH2, to afford Pd@MIL-101-NH2. The hydrophobic perfluoroalkyls were post-synthetically modified onto -NH2 group to yield Pd@MIL-101-Fx (x = 3, 5, 7, 11, 15), which engineer the MOF pore walls to regulate Pd surrounding microenvironment and interaction with substrates. As a result, both the dehydrogenation coupling of organosilane and hydrogenation of halogenated nitrobenzenes show that their activity and selectivity can be greatly promoted upon hydrophobic modification due to the favorable substrate enrichment and regulated interactions between Pd and the modified MOF hosts, far surpassing the traditional supported or surfactant-protected Pd NPs. We envision metal NPs@MOF composites would be an ideal platform integrating the inherent activity of well-accessible metal sites with engineered microenvironment via readily tunable MOFs. Regulating the interaction between active sites and substrates is of great importance in catalysis. The common strategy is to modify the surface of active sites (mostly, metal nanoparticles/NPs in heterogeneous catalysts) with diverse molecules, which, unfortunately, is unfavorable to substrate accessibility and, thus, detrimental to activity. Therefore, it is highly desired to develop heterogeneous catalysts featuring naked metal NPs, which are simultaneously able to regulate interaction with substrates. This puts forward long-standing contradictory challenges on metal NP-based catalysts: (1) exposed active sites, requiring naked metal surface, for their good accessibility; (2) functional molecules around active sites, affording tunable interaction with substrates, for enhanced activity and selectivity. To meet the above challenges, we judiciously encapsulate surface-naked metal NPs into MOFs, achieving tunable interaction with substrates by engineering the MOF pore wall microenvironment.