Experiments on Reaction of Polyethylene and Water under High Pressure and High Temperature
-
摘要: 在金刚石压腔设备中进行聚乙烯的高温高压裂解实验研究。实验分含水和不含水两种情况。在显微镜下观察反应过程中的变化并显微照相记录有关现象,在高压下就位测定反应过程中荧光的变化。用气相色谱方法测定气相产物组成。含水实验中CH4占烃类气体产物的92%并有CO2生成,固体残余物非常少,表明水直接参与了化学反应,为烃类气体的形成提供氢源,为CO2的形成提供氧源。不含水实验中烃类气体的产率相对较低并有较多的固相残余物存在。用热力学理论探讨了实验中有关反应的机制。根据聚乙烯与干酪根结构的可比性,推测在水参与条件下有利于提高有机质裂解成烃的产率。Abstract: Hydrous and anhydrous pyrolysis of polyethylene under high temperature and high pressure was conducted in diamond anvil cell (DAC) apparatus. Reaction phenomena can be observed by microscope and be recorded by micrography during the experimental processes. At the meantime, in situ fluorescence change can be determined under high pressure. Compositions of gas products were analyzed by gas chromatographic technique. It shows that CH4 make up about 92% of the total gas hydrocarbon products, CO2 and very little solid residue were existed in the hydrous pyrolysis experiment. The results indicate that H2O participates in the chemical reaction directly, offering H to hydrocarbons and O to CO2. Anhydrous pyrolysis of polyethylene generates less gas hydrocarbons and much more solid residue than hydrous run. Thermodynamic theory was used to discuss reaction mechanism in the experiments. Compared polyethylene structure with kerogen, we infer that the ratio of hydrocarbons generation would be increased while H2O exist in the organic matter pyrolysis processes.
-
Key words:
- polyethylene /
- H2O /
- fluorescence /
- gas chromatography /
- thermodynamics
-
Seewald J S. Evidence for Metastable Equilibrium between Hydrocarbons under Hydrothermal Conditions [J]. Nature, 1994, 370: 285-287. Seewald J S, Benttez-Nelson B C, Whelan J K. Laboratory and Theoretical Constraints on the Generation and Composition of Natural Gas [J]. Geochimica et Cosmochimica Acta, 1998, 62(9): 1599-1617. Lewan M D. Experiments on the Role of Water in Petroleum Formation [J]. Geochimica et Cosmochimica Acta, 1997, 61(17): 3691-3723. 傅家谟, 秦匡宗. 干酪根地球化学 [M]. 广州: 广东科技出版社, 1995. 翁克难, 肖万生, 张惠之, 等. 石墨、菱铁矿与超临界水反应的实验研究 [J].髙压物理学报, 1996, 10(4): 241-244. Deines P. The Carbon Isotopic Composition of Diamonds: Relationship to Diamond Shape, Color, Occurrence and Vapor Composition [J]. Geochimica et Cosmochimica Acta, 1980, 44: 943-961. Holloway J R. Graphite-CH4-H20-CO2 Equilibria at Low-Grade Metamorhpic Conditions [J]. Geology, 1984, 12: 455-458. 杨晓勇, 刘德良, 陶士振. 中国东部典型地幔岩中包裹体成分研究及意义 [J]. 石油学报, 1999, 20(1): 1923. 苏犁, 宋述光, 王志海. 北祁连山玉石沟地幔橄榄岩中富CH4流体包裹体及其意义 [J]. 科学通报, 1999, 44(8): 855-858. Hall D L, Bodnar R J. Methane in Fluid Inclusions from Granulites: A Product of Hydrogen Diffusion? [J]. Geochimica et Cosmochimica Acta, 1990, 54: 641-651. Saxena S K, Fei Y. High Pressure and High Temperature Fluid Fugacities [J]. Geochimica et Cosmochimica Acla, 1987, 51: 783-791. Belonochko B, Saxena S K. Equation of State of Fluid at High Temperature and Pressure [A]. Saxena S K. Thermo-dynamics and Estimation. Advances in Physical Geochemistry [C]. Springer-Verlag, 1992. 335-358. 林传仙, 白正华, 张哲儒. 矿物及有关化合物热力学数据手册 [M]. 北京: 科学出版社, 1985. Ancilotto F, et al. Dissociation of Methane into Hydrocarbons at Extreme (Planetary) Pressure and Temperalure [J]. Science, 1997, 275: 1288-1290. Benedetti L R, et al. Dissociation of CH4 at High Pressures and Temperatures: Diamond Formation in Giant Planet In-teriors? [J]. Science, 1999, 286: 100-102.
点击查看大图
计量
- 文章访问数: 8833
- HTML全文浏览量: 610
- PDF下载量: 607