科学研究

二氧化硅负载铂催化剂的制备及性能研究

展开
  • 1.湖北工业大学绿色轻工材料湖北省重点实验室,武汉430068;
    2.绿色轻质材料与加工湖北工业大学协同创新中心,武汉430068;
    3.湖北工业大学材料与化学工程学院,武汉430068;
    4.中国科学院化学研究所高技术材料实验室,北京100190
蔡诚(1995-),男,硕士研究生,主要从事有机硅材料的制备及性能研究。

网络出版日期: 2020-10-20

基金资助

湖北省自然科学基金(2016CFB205);湖北工业大学博士科研启动基金(BSQD14007)

Preparation and property of SiO2 supported Pt catalyst

Expand
  • 1.Hubei Provincial Key Laboratory of Green Materials for Light Industry,Hubei University of Technology,Wuhan 430068;
    2.Collaborative Innovation Center of Green Light-weight Materials and Processing,Hubei University of Technology,Wuhan 430068;
    3.School of Materials and Chemical Engineering,Hubei University of Technology,Wuhan 430068;
    4.Laboratory of Advanced Polymer Materials,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190

Online published: 2020-10-20

摘要

将乙烯基三乙氧基硅烷(VTES)改性的纳米SiO2与氯铂酸(H2PtCl6·6H2O)反应,通过乙烯基与Pt的络合作用制备SiO2负载Pt催化剂。对催化剂的Pt负载量和结构进行表征,探究了VTES与纳米SiO2质量比对催化剂Pt负载量的影响,并通过硅氢加成反应考察了催化剂的催化活性和重复利用性。结果表明,通过VTES改性的SiO2可以负载更多、更稳定的Pt催化剂。所制备的Pt/SiO2-Vi5催化剂Pt负载量为0.504%。将其用于二氯甲基硅烷与1-辛烯的硅氢加成反应中,当反应温度为80℃、反应5h时,转化率可达95.22%,β-加成产物的产率为95.11%,且催化剂至少可进行4次循环反应而催化活性无明显损失。

本文引用格式

蔡诚, 张志杰, 胡涛, 戴丽娜, 王浩宇, 吴崇刚, 龚兴厚 . 二氧化硅负载铂催化剂的制备及性能研究[J]. 化工新型材料, 2020 , 48(10) : 201 -205 . DOI: 10.19817/j.cnki.issn 1006-3536.2020.10.043

Abstract

SiO2 supported Pt catalysts were prepared via the reaction of nano-SiO2 modified by vinyltriethoxysilane(VTES) and chloroplatinic acid hexahydrate(H2PtCl6·6H2O) through the complexation between the vinyl groups and Pt.Pt content and structure of the catalysts were characterized.Effect of the mass ratio of VTES to SiO2 on Pt content were investigated,and the catalytic activity and recyclability of the catalyst were examined by a hydrosilylation reaction.Results showed that SiO2 modified by VTES could support more amount and stable Pt catalyst,with Pt content of the Pt/SiO2-Vi5 catalyst reached 0.504%.The Pt/SiO2-Vi5 catalyst displayed high activity in the hydrosilylation of dichloromethylsilane with 1-octene.When the reaction was conducted at 80℃ for 5h,the conversion of the reactant and yield of β-adduct reached 95.22% and 95.11%,respectively.Furthermore,the recovered catalyst could be recycled and reused for at least four times without any significant loss in activity.

参考文献

[1] 李光亮.有机硅高分子化学[M].北京:科学出版社, 1998:3-27.
[2] Hofmann R, VlatkoviAc'5 M, Wiesbrock F.Fifty years of hydrosilylation in polymer science:a review of current trends of low-cost transition-metal and metal-free catalysts, non-thermally triggered hydrosilylation reactions, and industrial applications[J].Polymers, 2017, 9(10):534.
[3] Nakajima Y, Shimada S.Hydrosilylation reaction of olefins:recent advances and perspectives[J].RSC Advances, 2015, 5(26):20603-20616.
[4] 马国维, 翁剑秀, 范宏.硅氢加成反应在功能有机硅化合物及材料中的应用[J].科技通报, 2012, 28(11):140-147.
[5] 萧斌, 李凤仪, 戴延凤.硅氢加成反应高选择性合成甲基苯乙基二氯硅烷[J].分子催化, 2006, 20(2):153-157.
[6] Speier J L.Homogeneous catalysis of hydrosilation by transition metals[J].Advances in Organometallic Chemistry, 1979, 17:407-447.
[7] Karstedt B.Platinum complexes of unsaturated siloxanes and platinum containing organopolysiloxanes:US, 3814730[P].1974-06-04.https://patents.google.com/patent/US3814730A/en.
[8] Pagliaro M, Ciriminna R, Pandarus V, et al.Platinum-based heterogeneously catalyzed hydrosilylation[J].European Journal of Organic Chemistry, 2013, 2013(28):6227-6235.
[9] Dioumaev V K, Bullock R M.A recyclable catalyst that precipitates at the end of the reaction[J].Nature, 2003, 424(6948):530.
[10] Xiao J, Qiu Z, He W, et al.Progress in platinum catalysts supported by inorganic carriers for hydrosilylation[J].Chinese Journal of Organic Chemistry, 2016, 36(5):987-999.
[11] 储诚灿, 苏朝晖.聚合物负载纳米材料及其在催化领域的应用[J].应用化学, 2016, 33(4):379-390.
[12] Rao F, Deng S, Chen C, et al.Graphite oxide-supported Karstedt catalyst for the hydrosilylation of olefins with triethoxysilane[J].Catalysis Communications, 2014, 46(5):1-5.
[13] Alonso F, Buitrago R, Moglie Y, et al.Hydrosilylation of alkynes catalysed by platinum on titania[J].Journal of Organometallic Chemistry, 2011, 696(1):368-372.
[14] Li F, Li Y.Preparation of efficient and environment-friendly silica-supported EDTA platinum catalyst and its applications in hydrosilylation of olefins and methyldichlorosilane[J].Journal of Molecular Catalysis A:Chemical, 2016, 420:254-263.
[15] Bai Y, Zhang S, Deng Y, et al.Use of functionalized PEG with 4-aminobenzoic acid stabilized platinum nanoparticles as an efficient catalyst for the hydrosilylation of alkenes[J].Journal of Colloid and Interface Science, 2013, 394:428-433.
[16] Zai H, Zhao Y, Chen S, et al.Heterogeneously supported pseudo-single atom Pt as sustainable hydrosilylation catalyst[J].Nano Research, 2018:1-9.
[17] Burneau A, Barres O, Gallas J P, et al.Comparative study of the surface hydroxyl groups of fumed and precipitated silicas[J].Langmuir, 1990, 6(8):1364-1372.
[18] Koch Carl C.Nanostructured materials:processing, properties, and applications[M].New York:Noyes Publications, 2002.
[19] Abad A, Corma A, García H.Catalyst parameters determining activity and selectivity of supported gold nanoparticles for the aerobic oxidation of alcohols:the molecular reaction mechanism[J].Chem A Eur J, 2008, 14(1):212-222.
[20] 杨辉, 陈飞.乙烯基三甲氧基硅烷对二氧化硅的超疏水改性研究[J].人工晶体学报, 2015, 44(9):2597-2605.
[21] Naumkin A V, Kraut-Vass A, Gaarenstroom S W, et al.NIST X-ray photoelectron spectroscopy database, NIST standard reference database 20, version 4.1[DB].Washington:US Department of Commerce, 2012.http://srdata.nist.gov/xps.
[22] Li J, Yang C, Zhang L, et al.A novel fumed silica-supported nitrogenous platinum complex as a highly efficient catalyst for the hydrosilylation of olefins with triethoxysilane[J].Journal of Organometallic Chemistry, 2011, 696(9):1845-1849.
Options
文章导航

/