[1]刘玉莹,王小琦,翟茂菁,等.甲烷催化裂解制备碳纳米管过程中二氧化碳的影响[J].南京师范大学学报(工程技术版),2020,20(02):066-71.[doi:10.3969/j.issn.1672-1292.2020.02.010]
　Liu Yuying,Wang Xiaoqi,Zhai Maojing,et al.Effect of CO2 on the Preparation of Carbon Nanotubesby Catalytic Cracking of CH4[J].Journal of Nanjing Normal University(Engineering and Technology),2020,20(02):066-71.[doi:10.3969/j.issn.1672-1292.2020.02.010]
点击复制

甲烷催化裂解制备碳纳米管过程中二氧化碳的影响
分享到：

南京师范大学学报（工程技术版）[ISSN:1006-6977/CN:61-1281/TN]

卷:
20卷
期数:
2020年02期
页码:
066-71
栏目:
化学工程与技术
出版日期:
2020-05-15

文章信息/Info

Title:
Effect of CO2 on the Preparation of Carbon Nanotubesby Catalytic Cracking of CH4
文章编号:
1672-1292(2020)02-0066-06
作者:
刘玉莹1; 2; 王小琦1; 2; 翟茂菁1; 2; 朱晓玮1; 2; 杨安宇1; 2; 董 艺1; 2; 蔡冰玉1; 2; 朴桂林1; 2; 王昕晔1; 2
(1.南京师范大学能源与机械工程学院,江苏 南京 210023)(2.南京师范大学江苏省物质循环与污染控制重点实验室,江苏 南京 210023)
Author(s):
Liu Yuying1; 2; Wang Xiaoqi1; 2; Zhai Maojing1; 2; Zhu Xiaowei1; 2; Yang Anyu1; 2; Dong Yi1; 2; Cai Bingyu1; 2; Piao Guilin1; 2; Wang Xinye1; 2
(1.School of Energy and Mechanical Engineering,Nanjing Normal University,Nanjing 210023,China)(2.Jiangsu Provincial Key Laboratory of Materials Cycling and Pollution Control,Nanjing Normal University,Nanjing 210023,China)
关键词:
沼气; 甲烷; 二氧化碳; 催化裂解; 镍; 碳纳米管
Keywords:
biogas; methane; carbon dioxide; catalytic cracking; nickel; carbon nanotube
分类号:
TQ546
DOI:
10.3969/j.issn.1672-1292.2020.02.010
文献标志码:
A
摘要:
生物质发酵沼气含有高浓度CH4,具有制备碳纳米管的潜力,但其中所含的大量CO2对碳纳米管制备存在潜在影响. 研究了CH4催化裂解制备碳纳米管过程中CO2的影响,使用商用Ni基催化剂和水平管式炉装置开展碳纳米管制备试验,采用TPR、TPO、SEM、TEM等手段对催化剂和碳纳米管进行表征. 650 ℃时催化裂解效率最高,碳产物最大质量为催化剂质量的4倍,其中主要产物为多壁碳纳米管. CO2对最佳催化裂解温度、催化裂解效率及多壁碳纳米管产量无显著影响,但CO2的存在增加了碳纳米管内外径、长度和平滑度. 这可能是由于CH4催化裂解产生无定形积碳,阻碍碳纳米管生长; 而CO2与积碳反应清除积碳,促进了碳纳米管生长. 从CO2的影响来看,沼气制备碳纳米管具有可行性.
Abstract:
Biogas contains high concentrations of CH4,so it has a potential to produce carbon nanotubes. However,the high concentration of CO2 in it has a potential impact on the preparation. In this paper,we investigate the effect of CO2 on the preparation of carbon nanotubes by catalytic cracking of methane. The carbon nanotube preparation experiments are carried out by using the commercial nickel-based catalyst and the horizontal tube furnace apparatus. The catalysts and carbon nanotubes are characterized by TPR,TPO,SEM,TEM,etc. The highest catalytic cracking efficiency is obtained at 650 ℃ with the maximum mass of carbon products which are 4 times as much as that of the catalyst. The main product is multi-walled carbon nanotubes. CO2 has no effect on the best temperature for catalytic cracking,the highest efficiency of catalytic cracking and the production of multi-wall carbon nanotubes. However,CO2 increases the inner diameter,length and smoothness of the carbon nanotubes,which may be due to the deposited amorphous carbon from CH4 inhibition of catalytic cracking,that hindered the growth of carbon can nanotubes. However,the reaction of CO2 and deposited carbon removes the deposited carbon,resulting in the enhancement of the carbon nanotubes growth. From the perspective of the impact of CO2,it is feasible to prepare carbon nanotubes from biogas.

参考文献/References:

[1] 张强,黄佳琦,赵梦强,等. 碳纳米管的宏量制备及产业化[J]. 中国科学:化学,2013,43(6):641-666.
[2]ROBERTSON S D. Carbon formation from methane pyrolysis over some transition metal surfaces—I. Nature and properties of the carbons formed[J]. Carbon,1970,8(3):365-374.
[3]胡晓阳. 碳纳米管和石墨烯的制备及应用研究[D]. 郑州:郑州大学,2013.
[4]CALGARO C O,PEREZ-LOPEZ O W. Graphene and carbon nanotubes by CH4 decomposition over Co-Al catalysts[J]. Materials Chemistry Physics,2019,226:6-19.
[5]YOO Y J,BAIK H K. Synthesis of carbon nanotubes by chemical vapor deposition technique[J]. Journal of Vacuum Science & Technology B,2001,19(1):27-31.
[6]BOROWIECKI T,GAC W,DENIS A. Effects of small MoO3 additions on the properties of nickel catalysts for the steam reforming of hydrocarbons:Ⅲ. Reduction of Ni-Mo/Al2O3 catalysts[J]. Applied Catalysis A:General,2004,270(1/2):27-36.
[7]SERRANO-LOTINA A,DAZA L. Highly stable and active catalyst for hydrogen production from biogas[J]. Journal of Power Sources,2013,238:81-86.
[8]AMACZ A. CNT and H2 production during CH4 decomposition over Ni/CeZrO2. I. A mechanistic study[J]. ChemEngineering,2019,3(1):26.
[9]周固民,冯永成,赵社涛,等. 程序升温氧化法测定碳纳米管的纯度[J]. 合成化学,2002,10(6):534-538.
[10]彭峰,王红娟,余皓,等. 用程序升温氧化技术研究碳纳米管氧化动力学[J]. 石油化工,2005,34(11):1064-1067.
[11]孔令涌,罗文耀,欧阳增图,等. 浅析碳纳米管纯度测定方法[J]. 材料导报,2006,20(增刊1):114-116.
[12]周蕾. 多壁碳纳米管的改性及其吸附性能研究[D]. 长沙:中南大学,2013.
[13]赵江. 高质量多壁碳纳米管的制备方法和应用研究[D]. 上海:上海交通大学,2013.
[14]宋晓瑜. 多壁碳纳米管的功能化及应用[D]. 大连:大连理工大学,2013.
[15]TAN P J,GAO Z H,SHEN C F,et al. Ni-Mg-Al solid basic layered double oxide catalysts prepared using surfactant-assisted coprecipitation method for CO2 reforming of CH4[J]. Chinese Journal of Catalysis,2014,35(12):1955-1971.
[16]李琳,张露明,张煜华,等. 镍负载量对Ni/MgO(111)催化甲烷二氧化碳重整反应性能影响[J]. 燃料化学学报,2015,43(3):315-322.
[17]方修忠. 高效抗积碳Ni基甲烷重整制氢催化剂的制备和性能研究[D]. 南昌:南昌大学,2016.

相似文献/References:

[1]林 峰,李传统.生物质厌氧发酵动力学模型分析[J].南京师范大学学报(工程技术版),2013,13(03):057.
　Lin Feng,Li Chuantong.Analysis of the Kinetic Model of Biomass Anaerobic Fermentation[J].Journal of Nanjing Normal University(Engineering and Technology),2013,13(02):057.
[2]王昕晔,李静漪,杜 荣,等.CO/CH4在Ni(111)表面协同催化裂解机制[J].南京师范大学学报(工程技术版),2019,19(01):072.[doi:10.3969/j.issn.1672-1292.2019.01.010]
　Wang Xinye,Li Jingyi,Du Rong,et al.Mechanisms on Synergetic Catalysis Crackingof CO/CH4 on Ni(111)[J].Journal of Nanjing Normal University(Engineering and Technology),2019,19(02):072.[doi:10.3969/j.issn.1672-1292.2019.01.010]

备注/Memo

备注/Memo:
收稿日期:2019-08-20.
基金项目:中国博士后科学基金项目(2017M621778)、江苏省高校自然科学研究面上项目(17KJB470007)、江苏省博士后科研资助计划项目(1701160B).
通讯作者:王昕晔,博士,副教授,研究方向:化石燃料清洁利用. E-mail:xinye.wang@njnu.edu.cn
更新日期/Last Update: 2020-05-15