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  

Study on MWCNTs@Fe3O4@Rh for NBR hydrogenation

作　　者：姚含波 钱家盛[1] 夏茹[1] 苗继斌[1] 杨斌[1] 曹明[1] Yao Hanbo;Qian Jiangsheng;Xia Ru;Miao Jinbin;Yang Bin;Cao Ming(Anhui Province Key Laboratory of Environment-friendly Polymer Materials,School ofChemistry &Chemical Engineering,Anhui University,Hefei 230601)

机构地区：[1]安徽省绿色高分子材料重点实验室安徽大学化学化工学院

出　　处：《化工新型材料》2019年第7期204-208,共5页New Chemical Materials

基　　金：国家自然科学基金(51273001)

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C=C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%。Fe3O4particles 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 Fe3O4nanoparticles with diameter of 300~400nm,and the surface loaded Rh nanoparticles with diameter less than 10nm.The Rh nanoparticles and Fe3O4nanoparticles had a better load on the surface of the carbon nanotube.The existence of Fe3O4and 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@[e-mail] conversion of 98.17% and good selectivitytor C=C 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 3times,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 

分 类 号：TQ426[化学工程] TQ333.7