Ni_2O_3/NH_4Cl复合催化体系催化聚丙烯/稻壳共混物制备竹节状碳纳米管的研究
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摘要
用催化碳化聚丙烯/稻壳共混物的方法制备了竹节状碳纳米管。首先制备含有稻壳粉、氧化镍(Ni_2O_3)、氯化铵(NH_4Cl)的聚丙烯共混物;然后在氮气保护下,通过一步碳化共混物的方法制备出竹节状碳纳米管。采用扫描电子显微镜、透射电子显微镜、X射线衍射仪、拉曼光谱和热重分析仪等对所得碳纳米管的形貌、微观结构、相结构、石墨化度和热稳定性进行表征。结果表明:复合催化剂(Ni_2O_3和NH_4Cl)是获得高产率碳纳米管的关键因素;同时稻壳粉助剂对生成竹节状碳纳米管有重要影响;所得竹节状碳纳米管直径在10 nm左右,长度在几百纳米至几微米范围内。该研究提供一种新的潜在回收利用废旧塑料的方法。
Bamboo-like carbon nanotubes were prepared by catalytic carbonization of polypropylene/rice husk blends. Polypropylene blends containing rice husk powder, nickel oxide(Ni_2O_3) and ammonium chloride(NH_4Cl) were prepared. Then bamboo-shaped carbon nanotubes were prepared by one-step carbonization under nitrogen protection. The morphology, microstructure, phase structure, graphitization degree and thermal stability of carbon nanotubes were characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, Raman spectroscopy and thermogravimetric analysis. The results show that composite catalysts(Ni_2O_3 and NH_4Cl) are the key factors to obtain high yield carbon nanotubes; rice husk powder additives have an important influence on the formation of bamboo carbon nanotubes; the diameter of the obtained bamboo carbon nanotubes is about 10 nm, and the length of the bamboo carbon nanotubes is in the range of several hundred nanometers to several micrometers. This study provides a new potential method for recycling waste plastics.
Bamboo-like carbon nanotubes were prepared by catalytic carbonization of polypropylene/rice husk blends. Polypropylene blends containing rice husk powder, nickel oxide(Ni_2O_3) and ammonium chloride(NH_4Cl) were prepared. Then bamboo-shaped carbon nanotubes were prepared by one-step carbonization under nitrogen protection. The morphology, microstructure, phase structure, graphitization degree and thermal stability of carbon nanotubes were characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, Raman spectroscopy and thermogravimetric analysis. The results show that composite catalysts(Ni_2O_3 and NH_4Cl) are the key factors to obtain high yield carbon nanotubes; rice husk powder additives have an important influence on the formation of bamboo carbon nanotubes; the diameter of the obtained bamboo carbon nanotubes is about 10 nm, and the length of the bamboo carbon nanotubes is in the range of several hundred nanometers to several micrometers. This study provides a new potential method for recycling waste plastics.
引文
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[2]Wu C,Wang Z,Wang L,et al.Sustainable processing of waste plastics to produce high yield hydrogen-rich synthesis gas and high quality carbon nanotubes[J].Rsc Advances,2012,2(10):4 045-4 047.
[3]Wu C,Williams P T.Pyrolysis-gasification of plastics,mixed plastics and real-world plastic waste with and without NiMg-Al catalyst[J].Fuel,2010,89(10):3 022-3 032.
[4]Serrano D P,Aguado J,Escola J M.Developing advanced catalysts for the conversion of polyolefinic waste plastics into fuels and chemicals[J].ACS Catal,2012,2(9):1 924-1 941.
[5]Al-Salem S M,Lettieri P,Baeyens J.Recycling and recovery routes of plastic solid waste(PSW):A review[J].Waste Management,2009,29(10):2 625-2 643.
[6]Acomb J C,Wu C,Williams P T.Control of steam input to the pyrolysis-gasification of waste plastics for improved production of hydrogen or carbon nanotubes[J].Applied Catalysis B:Environmental,2014,147:571-584.
[7]Tang T,Chen X,Meng X,et al.Synthesis of multiwalled carbon nanotubes by catalytic combustion of polypropylene[J].Angewandte Chemie,2005,44(10):1 517-1 520.
[8]Jiang G,Yao K,Jie L,et al.Catalytic conversion of linear low density polyethylene into carbon nanomaterials under the combined catalysis of Ni2O3,and poly(vinyl chloride)[J].Chemical Engineering Journal,2013,215-216(3):339-347.
[9]Jiang G,Liu J,Jiang Z,et al.Striking influence of chain structure of polyethylene on the formation of cupstacked carbon nanotubes/carbon nanofibers under the combined catalysis of CuBr and NiO[J].Applied Catalysis B:Environmental,2014,147(1):592-601.
[10]Song R,Ji Q.Synthesis of carbon nanotubes from polypropylene in the presence of Ni/Mo/MgO catalysts via combustion[J].Chemistry Letters,2011,40(10):1 110-1 112.
[11]Song R,Liu L,Yan D,et al.A method for the direct growth of carbon nanotubes on macroscopic carbon substrates[J].Journal of Materials Science,2016,51(5):2 330-2 337.
[12]Li G,Tan S,Song R,et al.Synergetic effects of molybdenum and magnesium in Ni-Mo-Mg catalysts on the one-step carbonization of polystyrene into carbon nanotubes[J].Industrial&Engineering Chemistry Research,2017,56(41):11 734-11 744.
[13]Xu T T,Fisher F T,And L C B,et al.Bone-shaped nanomaterials for nanocomposite applications[J].Nano Letters,2003,3(8):1 135-1 139.
[14]Saito Y,Yoshikawa T.Bamboo-shaped carbon tube filled partially with nickel[J].Journal of Crystal Growth,1993,134(1):154-156.
[15]Chen Y,Shaw D T,Guo L.Field emission of different oriented carbon nanotubes[J].Applied Physics Letters,2000,76(17):2 469-2 471.
[16]Lee C J,Park J.Growth model for bamboolike structured carbon nanotubes synthesized using thermal chemical vapor deposition[J].J Phys Chem B,2001,105(12):2 365-2 368.
[17]Li Y F,Qiu J S,Zhao Z B,et al.Bamboo-shaped carbon tubes from coal[J].Chemical Physics Letters,2002,366(5):544-550.
[18]González I,De J J,Ca?izales E.Bamboo-shaped carbon nanotubes generated by methane thermal decomposition using Ni nanoparticles synthesized in water-oil emulsions[J].Micron,2011,42(8):819-825.
[19]Zhang X X,Li Z Q,Wen G H,et al.Microstructure and growth of bamboo-shaped carbon nanotubes[J].Chemical Physics Letters,2001,333(6):509-514.
[20]Liu J,Shao M,Chen X,et al.Large-scale synthesis of carbon nanotubes by an ethanol thermal reduction process[J].Journal of the American Chemical Society,2003,125(27):8 088-8 089.
[21]Wu X,Tao Y,Lu Y,et al.High-pressure pyrolysis of melamine route to nitrogen-doped conical hollow and bamboo-like carbon nanotubes[J].Diamond&Related Materials,2006,15(1):164-170.
[22]Deepak F L,John N S,Govindaraj A,et al.Nature and electronic properties of Y-junctions in CNTs and N-doped CNTs obtained by the pyrolysis of organometallic precursors[J].Chemical Physics Letters,2005,411(4-6):468-473.
[23]Liu H,Zhang Y,Li R,et al.Structural and morphological control of aligned nitrogen-doped carbon nanotubes[J].Carbon,2010,48(5):1 498-1 507.