Synthesis of Bamboo-like N-doped Carbon Nanotubes by Catalytic Pyrolysis of Melamine
摘 要
以三聚氰胺为原料、FeCl2·6H2O为催化剂前驱体,应用催化热解法制备竹节状氮掺杂碳纳米管,研究了反应温度和FeCl2·6H2O添加量对产物物相组成和显微结构的影响。结果表明:当反应温度为650~800℃时,碳纳米管的生成量及长径比均随反应温度的升高先增后降,其最佳反应温度为750℃;在750℃热解时,随着FeCl2·6H2O添加量的增加,碳纳米管的生成量和长径比均先增后减,最佳添加量为三聚氰胺质量的0.50%,在此条件下合成的碳纳米管直径为40~50 nm,长度为10~15 μm,碳纳米管中氮掺杂量(原子分数)为3.42%,其中石墨型氮的物质的量分数为43.1%。
Abstract
Bamboo-like N-doped carbon nanotubes were prepared by catalytic pyrolysis method with melamine as raw material and FeCl2·6H2O as catalyst precursor. The effects of the reaction temperature and FeCl2·6H2O content on the phase composition and microstructure of the product were investigated. The results show that at the reaction temperatures of 650-800℃, the yield and length to diameter ratio of the carbon nanotubes first increased and then decreased with the increase of reaction temperature. The optimal reaction temperature was 750℃. When pyrolyzing at 750℃, the yield and length to diameter ratio of the carbon nanotubes first increased and then decreased with the increase of FeCl2·6H2O content and the optimal content was 0.50wt% of melamine. The obtained carbon nanotubes under this condition had diameters of 40-50 nm and lengths of 10-15 μm, the N-doping amount in the carbon nanotubes was about 3.42at%, in which the fraction of graphitic N was about 43.1mol%.
中图分类号 TB321 DOI 10.11973/jxgccl201804006
所属栏目 新材料 新工艺
基金项目 国家自然科学基金面上项目(51472184,51472185);湖北省教育厅高等学校优秀中青年科技创新团队计划项目(T201602)
收稿日期 2017/7/30
修改稿日期 2018/3/7
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备注郑扬帆(1994-),女,湖北宜昌人,硕士研究生
引用该论文: ZHENG Yangfan,LIANG Feng,TIAN Liang,WANG Junkai,ZHANG Haijun. Synthesis of Bamboo-like N-doped Carbon Nanotubes by Catalytic Pyrolysis of Melamine[J]. Materials for mechancial engineering, 2018, 42(4): 27~30
郑扬帆,梁峰,田亮,王军凯,张海军. 催化热解三聚氰胺合成竹节状氮掺杂碳纳米管[J]. 机械工程材料, 2018, 42(4): 27~30
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【4】王利军, 解丽丽, 李永伦,等. 氮掺杂竹节状碳纳米管的催化合成[J]. 化学学报, 2007, 65(10):913-916.
【5】ZHOU K, SI J, JIA J, et al. Reactivity enhancement of N-CNTs in green catalysis of C2H2 hydrochlorination by a Cu catalyst[J]. RSC Advances, 2014, 4(15):7766-7769.
【6】ILINICH G N, MOROZ B L, RUDINA N A, et al. Growth of nitrogen-doped carbon nanotubes and fibers over a gold-on-alumina catalyst[J]. Carbon, 2012, 50(3):1186-1196.
【7】罗志虹, 朱其峰, 黄业富,等. 氮掺杂碳纳米管的制备及其应用[J]. 材料导报, 2016, 30(5):138-143.
【8】GOLBERG D, DOROZHKIN P, BANDO Y, et al. Semiconducting B-C-N nanotubes with few layers[J]. Chemical Physics Letters, 2002, 359(3/4):220-228.
【9】LEE Y T, KIM N S, BAE S Y, et al. Growth of vertically aligned nitrogen-doped carbon nanotubes:Control of the nitrogen content over the temperature range 900-1100℃[J]. The Journal of Physical Chemistry B, 2003, 107(47):12958-12963.
【10】SEN R, SATISHKUMAR B C, GOVINDARAJ A, et al. B-C-N, C-N and B-N nanotubes produced by the pyrolysis of precursor molecules over Co catalysts[J]. Chemical Physics Letters, 1998, 287(5/6):671-676.
【11】HOU P X, SONG M, LI J C, et al. Synthesis of high quality nitrogen-doped single-wall carbon nanotubes[J]. Science China Materials, 2015,58(8):603-610.
【12】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, 2015, 411(4/5/6):468-473.
【13】BARZEGAR H R, GRACIAESPINO E, SHARIFI T, et al. Nitrogen doping mechanism in small diameter single-walled carbon nanotubes:Impact on electronic properties and growth selectivity[J]. The Journal of Physical Chemistry C, 2017, 117(48):25805-25816.
【14】CHEN Y, SHAW D T, GUO L. Field emission of different oriented carbon nanotubes[J]. Applied Physics Letters, 2000, 76(17):2469-2471.
【15】LEE C J, PARK J. Growth model for bamboolike structured carbon nanotubes synthesized using thermal chemical vapor deposition[J]. The Journal of Physical Chemistry B, 2001, 105(12):2365-2368.
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