丙烯在模型孔中CVI过程的热解炭沉积

汤哲鹏; 李爱军; 李照谦; 彭雨晴

丙烯在模型孔中CVI过程的热解炭沉积

1.
上海大学材料复合及先进分散技术教育部工程中心, 上海 200072;
2.
上海航天设备制造总厂, 上海 200245

基金项目: 教育部博士点基金（20113108120019）；上海人才发展资金（2011028）；航空基金（2013ZFS6001）；上海市科委基金（13521101202）.

详细信息

作者简介:
汤哲鹏,博士研究生.E-mail:tangzhepong@shu.edu.cn

通讯作者:
彭雨晴,博士.E-mail:yuqing14@shu.edu.cn

中图分类号: TB332
计量
- 文章访问数: 413
- HTML全文浏览量: 148
- PDF下载量: 242
- 被引次数: 0
出版历程
- 收稿日期: 2017-07-08
- 录用日期: 2017-11-13
- 修回日期: 2017-10-09
- 刊出日期: 2017-10-28

Chemical vapor infiltration of pyrocarbon from propene into model capillaries

1.
School of Materials Science and Engineering, Shanghai University, Shanghai 200072, China;
2.
Shanghai Aerospace Equipment Manufacturer, Shanghai 200245, China

Funds: Doctoral Fund of Ministry of Education (20113108120019); Shanghai talent development fund (2011028); Aviation fund (2013ZFS6001); Shanghai Committee of Science and Technology (13521101202).

摘要

摘要: 本文在温度为1 223 K，总压强40 kPa （N₂：C₃H₆=9：1）和停留时间0.56 s下，以丙烯为前驱体在内径为1.0 mm和长度31.0 mm的模型孔中裂解沉积生成热解炭。以15 h为沉积周期经75 h沉积实验得到最终试样，通过制样观察热解炭沿模型孔长度方向的沉积厚度，分析在基底水平和垂直方向上热解炭的沉积速率变化。结果表明，在该实验条件下热解炭沿模型孔长度方向由孔口到末端的沉积速率降低；而在垂直方向位置较低处的模型孔，热解炭沿长度方向的沉积速率梯度较小。通过耦合丙烯的均气相反应机理和总括反应机理，对该实验条件下丙烯在模型孔中的热解炭沉积过程进行模拟。在平推流反应器模型中，运用均气相反应机理对丙烯裂解的气相组分变化进行模拟，并将平推流反应器相应位置的气体组分浓度作为对应模型孔入口的初始浓度。运用总括反应机理的热解炭沉积模型，对丙烯在模型孔中的化学气相渗透过程进行模拟。对照热解炭在模型孔中沉积厚度的实验结果，证明该模型的合理性。模拟和实验结果表明通过减少气体停留时间可适当减缓热解炭表面封孔现象。
- 热解炭 /
- 丙烯 /
- 化学气相渗透 /
- 模型孔 /
- 模拟
Abstract: 7 dead-end parallel capillaries 1.0 mm in diameter, 31.0 mm in length and 10 mm separation were aligned perpendicular to the axis of a gas conducting tube and infiltrated at 1 223 K and 40 kPa (N₂:C₃H₆=9:1) for 75 h with a gas residence time of 0.56 s within the tube. The thickness of the pyrocarbon layers produced was determined along each capillary at 15h intervals. Results indicate that the pyrocarbon deposition rate decreases from the mouth to the end of the capillaries and the rate gradients are lower in the capillaries nearer to the gas inlet. Pyrocarbon deposition in the capillaries was simulated by a deposition model using the lumped reaction mechanism. The gas composition in the capillary mouths was obtained from computation by assuming that gas-phase reactions are homogeneous and the tube is a plug flow reactor. The calculated deposition rate profiles agree well with the experimental ones. Both the experimental and theoretical results indicate that pore blockage is relieved by reducing the gas residence time within the conducting tube.
- Pyrocarbon /
- Propene /
- Chemical Vapor Infiltration /
- Capillary /
- Modeling

HTML全文

下载: 全尺寸图片幻灯片

参考文献(28)

Fitzer E. Manocha L M. Carbon Reinforcements and Carbon/Carbon Composites[M]. Berlin, Heidelberg:Springer, 1998.

Golecki I. Rapid vapor-phase densification of refractory composites[J]. Mat Sci Eng R, 1997, 20(2):37-124.

Delhaes P. Chemical vapor deposition and infiltration processes of carbon materials[J]. Carbon, 2002, 40(5):641-657.

Oberlin A. Pyrocarbons[J]. Carbon, 2002, 40(1):7-24.

Zhang W, Hüttinger K J. Simulation studies on chemical vapor infiltration of carbon[J]. Compos Sci Technol, 2002, 62(15):1947-1955.

Hu Z, Hüttinger K J. Chemical vapor infiltration of carbon-revised, Part Ⅱ:Experimental results[J]. Carbon, 2001, 39(7):1023-1032.

Zhang W, Hüttinger K J. Chemical vapor infiltration of carbon-revised, Part I:Model simulations[J]. Carbon, 2001, 39(7):1013-1022.

Hu Z, Schoch G, Hüttinger K J. Chemistry and kinetics of chemical vapor infiltration of Pyrocarbon:VⅡ:infiltration of capillaries of equal size[J]. Carbon, 2000, 38(7):1059-1065.

张伟刚. 化学气相沉积-从烃类气体到固体炭[M]. 北京:科学出版社,2007:20-120. (Zhang W. Chemical Vapor Deposition-From Hydrocarbon Gas to Solid Carbon[M]. Beijing:Science Press, 2007:20-120.)

Dong G, Hüttinger K J. Consideration of reaction mechanisms leading to pyrolytic carbon of different textures[J]. Carbon, 2002, 40(14):2515-2528.

Xu W, Zhang Z, Bai R, et al. Kinetic Modeling of Gas-Phase Reactions for CVD from Propane[J]. New Carbon Mater, 2014, 29:67-77.

Lacroix R, Fournet R, Ziegler D I, et al. Kinetic modeling of surface reactions involved in CVI of Pyrocarbon obtained by propane pyrolysis[J]. Carbon, 2010, 48(1):132-144.

Tang Z, Li A, Zhang Z, et al. Chemistry and Kinetics of Heterogeneous Reaction Mechanism for Chemical Vapor Infiltration of Pyrolytic Carbon from Propane[J]. Ind Eng Chem Res, 2014, 53(45):17537-17546.

Kee R J, Coltrin M E, Glarborg P. Chemically Reacting Flow:Theory and Practice[M]. A John Wiley and Sons:New Jersey, 2003.

Li A, Deutschmann O. Transient modeling of chemical vapor infiltration of methane using multi-step reaction and deposition models[J]. Chem Eng Sci, 2007, 62(18-20):4976-4982.

Li A, Norinaga K, Zhang W, Deutschmann O. Modeling and simulation of materials synthesis:Chemical vapor deposition and infiltration of pyrolytic carbon[J]. Compos Sci Technol, 2008, 68(5):1097-1104.

Li H, Li A, Bai R, Li K. Numerical simulation of chemical vapor infiltration of propylene into C/C composites with reduced multi-step kinetic models[J]. Carbon, 2005, 43(14):2937-2950.

Benzinger W H, Hüttinger K J. Chemistry and kinetics of chemical vapor infiltration of Pyrocarbon:IV. Investigation of methane/hydrogen mixtures[J]. Carbon, 1999, 37(6):931-940.

Benzinger W H, Hüttinger K J. Chemistry and kinetics of chemical vapor deposition of Pyrocarbon:Ⅲ. Pyrocarbon deposition from ethylene, acetylene and 1,3-butadiene in the low temperature regime[J]. Carbon, 1998, 36(3), 11.

Vignoles G L, Goyheneche J, Sebastian P, et al. The film-boiling densification process for C/C composites fabrication:from local scale to overall optimization[J]. Chem Eng Sci, 2006, 61(17):5636-5653.

Vignoles G L. Modelling of the CVI processes[J]. Adv Sci Technol, 2006, 50:97-106.

Norinaga K, Deutschmann O. Detailed Kinetic Modeling of Gas-Phase Reactions in the Chemical Vapor Deposition of Carbon from Light Hydrocarbons[J]. Ind Eng Chem Res, 2007, 46(11):3547-3557.

Norinaga K, Janardhanan V M, Deutschmann O. Detailed chemical kinetic modeling of pyrolysis of ethylene, acetylene, and propylene at 1073-1373 K with a plug-flow reactor model[J]. Int J Chem Kinet, 2008, 40(4):199-208.

enzinger W H, Hüttinger K J. Chemistry and kinetics of chemical vapor infiltration of pyrocarbon:VI. Mechanical and structural properties of infiltrated carbon fiber felt[J]. Carbon, 1999, 37(8):1311-1322.

Zhang W, Hu Z, Hüttinger K J. Chemical vapor infiltration of carbon fiber felt:optimization of densification and carbon microstructure[J]. Carbon, 2002, 40(14):2529-2545.

Zhang W, Hüttinger K J. Densification of a 2D carbon fiber preform by isothermal, isobaric CVI:Kinetics and carbon microstructure[J]. Carbon, 2003, 41(12):2325-2337.

Deutschmann O, Tischer S, Correa C, et al. DETCHEM Software Package 2.1 Ed[M], 2007.

Isabelle Z D, Fournet R, Marquaire P M. Pyrolysis of propane for CVI of Pyrocarbon, Part Ⅲ:Experimental and modeling study of the formation of Pyrocarbon[J]. J Anal Appl Pyrol, 2007, 79(1-2):268-277.

施引文献

资源附件(0)

访问统计