磁性碳纳米管负载铑催化剂在丁腈橡胶氢化方面的应用研究

姚含波, 钱家盛*, 夏茹, 苗继斌, 杨斌, 曹明

化工新型材料 ›› 2019, Vol. 47 ›› Issue (7) : 204 -208.

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化工新型材料 ›› 2019, Vol. 47 ›› Issue (7) : 204-208.
科学研究

磁性碳纳米管负载铑催化剂在丁腈橡胶氢化方面的应用研究

    姚含波, 钱家盛*, 夏茹, 苗继斌, 杨斌, 曹明
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Study on MWCNTs@Fe3O4@Rh for NBR hydrogenation

  • Yao Hanbo, Qian Jiangsheng, Xia Ru, Miao Jinbin, Yang Bin, Cao Ming
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摘要

采用水热合成法,在多壁碳纳米管(MWCNTs)表面原位生成四氧化三铁(Fe3O4)纳米粒子,制备碳纳米管磁性载体(MWCNTs@Fe3O4),再将铑(Rh)纳米粒子负载在该磁性载体上,形成新型磁性碳纳米管催化剂(MWCNTs@Fe3O4@Rh)。采用透射电子显微镜(TEM),X-射线粉末衍射(XRD),X射线光电子能谱(XPS)等手段表征催化剂的结构和形貌,从TEM可以看出碳纳米管缠绕在直径300nm~400nm的四氧化三铁(Fe3O4)纳米粒子上,并且表面负载有直径小于10nm的Rh纳米粒子。采用XRD和XPS等手段也证明Fe3O4以及Rh粒子的存在。同时对该催化剂在丁腈橡胶(NBR)选择性加氢方面进行探索。在120℃,4.0MPa,8h条件下,得到了氢化率达到98.17%的氢化丁腈橡胶(HNBR),该催化剂对CC双键具有良好的选择性。将制备的MWCNTs@Fe3O4@Rh催化剂与传统的MWCNTs负载Rh的催化剂(MWCNTs@Rh)进行循环使用,发现在重复3次之后,新型催化剂仍能达到91.53%以上的氢化度,而传统的催化剂不到40%。

Abstract

Fe3O4 particles were combined with multi-walled carbon nanotubes(MWCNTs) to form MWCNTs@Fe3O4 magnetic carrier by in-situ method.Rhodium nanoparticles were loaded onto surface of magnetic carbon nanotubes to form MWCNTs@Fe3O4@Rh magnetic carbon nanotube catalysts.The structure and morphology of the catalyst were characterized by TEM,XRD and XPS.It can be seen from TEM that the carbon nanotubes were entangled in Fe3O4 nanoparticles with diameter of 300~400nm,and the surface loaded Rh nanoparticles with diameter less than 10nm.The Rh nanoparticles and Fe3O4 nanoparticles had a better load on the surface of the carbon nanotube.The existence of Fe3O4 and Rh particles can be demonstrated by powder X-ray diffraction(XRD) and X-ray photoelectron spectroscopy(XPS).The hydrogenation of nitrile butadiene rubber (NBR) was used to evaluate the catalytic properties of MWCNTs@Fe3O4@Rh.The conversion of 98.17% and good selectivity tor CC were obtained under optimum condition (120℃,4.0MPa,8h).In addition,the traditional catalyst loaded on carbon nanotubes directly(MWCNT@Rh) and prepared MWCNTs@Fe3O4@Rh catalyst were both recycled.After repeating 3 times,the hydrogenation degree of catalysts prepared still remain was 91.53%,while the hydrogenation degree of original catalyst was less than 40%.

关键词

丁腈橡胶 / 氢化 / 磁性碳纳米管

Key words

NBR / hydrogenation / magnetic carbon nanotube

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引用格式 ▾
磁性碳纳米管负载铑催化剂在丁腈橡胶氢化方面的应用研究[J]. 化工新型材料, 2019, 47(7): 204-208 DOI:

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参考文献

[1] Han K Y,Zuo H R,Zhu Z W,et al.High performance of palladium nanoparticles supported on carbon nanotubes for the hydrogenation of commercial polystyrene[J].Industrial & Engineering Chemistry Research,2013,52(50):17750-17759.
[2] Maheshwari S,Michael Tsapatsis A,Bates F S.Synthesis and thermodynamic properties of poly(cyclohexylethylene-b-dimethylsiloxane-b-cyclohexylethylene)[J].Macromolecules,2007,40(18):6638-6646.
[3] 周淑芹,姚明,徐瑞清,等.铑钌双金属双配体催化剂制备氢化丁腈橡胶[J].北京化工大学学报(自然科学版),2002,29(4):17-19.
[4] 周淑芹,姚明,岳冬梅,等.一种新型催化剂制备氢化丁腈橡胶的研究[J].高分子材料科学与工程,2002,18(5):69-72.
[5] 许贵显,周淑芹,岳冬梅,等.加氢催化剂,其制法及在不饱和共聚物加氢中的应用:中国,CN1263111[P].2000-08-16.
[6] Wei Z,Wu J,Pan Q,et al.Direct catalytic hydrogenation of an acrylonitrile-butadiene rubber latex using wilkinson's catalyst[J].Macromolecular Rapid Communications,2010,26(23):1768-1772.
[7] Yin L,Wei Z,Pan Q,et al.Hydrogenation of acrylonitrile-butadiene rubber latex using in situ synthesized RhCl(PPh3)3,catalyst[J].Applied Catalysis A General,2013,457(16):62-68.
[8] Yang L,Pan Q,Rempel G L.Development of a green separation technique for recovery of wilkinson's catalysts from bulk hydrogenated nitrile butadiene rubber[J].Catalysis Today,2013,207(207):153-161.
[9] Liu Y,Kim H,Pan Q,et al.Hydrogenation of acrylonitrile-butadiene copolymer latex using water-soluble rhodium catalysts[J].Catalysis Science & Technology,2013,3(10):2689-2698.
[10] Yang L,Wang H,Rempel G L,et al.Recovery of wilkinson's catalyst from hydrogenated nitrile butadiene rubber latex nanoparticles[J].Topics in Catalysis,2014,57(17/20):1558-1563.
[11] Piya-Areetham P,Prasassarakich P,Rempel G L.Organic solvent-free hydrogenation of natural rubber latex and synthetic polyisoprene emulsion catalyzed by water-soluble rhodium complexes[J].Journal of Molecular Catalysis A Chemical,2013,372(3):151-159.
[12] Horikoshi R,Kobayashi Y,Kageyama H.Illustrating catalysis with interlocking building blocks:a ruthenium carbene complex for olefin metathesis reactions[J].J Chem Educ,2014,91(2):255-258.
[13] Yamashita T,Hayes P.Analysis of XPS spectra of Fe2+,and Fe3+,ions in oxide materials[J].Applied Surface Science,2008,254(8):2441-2449.
[14] Cao P,Ni Y,Zou R,et al.Enhanced catalytic properties of rhodium nanoparticles deposited on chemically modified SiO2 for hydrogenation of nitrile butadiene rubber[J].Rsc Advances,2014,5(5):3417-3424.

基金资助

国家自然科学基金(51273001)

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