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水合物合成动力学实验及力学—化学耦合分析模型研究

Study of Kinetics Experiment and Mechanics-Chemistry Coupling Analysis Model for Hydrate Formation

【作者】 石定贤

【导师】 赵阳升;

【作者基本信息】 太原理工大学 , 工程力学, 2005, 硕士

【摘要】 近200年的水合物研究历史,其核心一直离不开对水合物形成和抑制机制的研究及应用,而其直接目的便是探寻更加经济和合理的形成与抑制方式。在对抑制剂的研究取得突破性进展之后,对其形成条件的优化便提到了首要位置。而研究水合物合成的宏观动力学条件对其生长的具体影响,探寻水合物生长过程中力学-化学耦合作用的微观机理,进一步优化其形成的外部条件也必然成为水合物技术应用研究的重中之重。 本文在广泛研究晶体成核理论和水合物生长经典动力学模型的基础上,应用新型的喷射实验平台对水合物制备过程中的宏观动力学条件,包括温度、压力、活性剂和气—水混合方式等对水合物成核、生成过程中的具体影响进行了对比试验,并针对实验现象,结合SLOAN的气-水簇成核理论,就水合物生长过程的微观机理进行了初步分析。研究表明,压力是控制水合物生长的关键因素,过冷、过压明显加快水合物成核过程,活性剂、喷射雾化方式能有效提高水合物生长速度,降低能耗。实验证明:基于喷射的水合物制备平台,相对常规搅拌方式而言,无论是生长速度还是最终含气量,都有了显著提高。 结合晶体生长理论和相关实验数据,本文建立了喷射雾化条件下水合物生长的力学-化学耦合计算模型。通过深入分析低温高压条件下气液间相互作用的力学机制与水合物生长的化学反应过程之间的耦合机理,综合考虑雾化方式、过饱和度、传质条件以及不同成核方式等对水合物生长过程的微观影响,建立起能够准确表达半间歇式雾化反应体系中水合物晶体生长与气水消耗的数学关联式,为雾化条件下水合物生长的微观机理研究提供理论支持。

【Abstract】 It has been 200 years for the hydrat studies so far, and the research directiones mainly concentrate on the study and application of the formation and inhibition mechanism. Its direct purpose is to get a more economical and effective formation or inhibition conditions .After the revolutionized success get in research of the inhibition, the chief problem turns to be the optimization of formation conditions. It has inevitably become the most important aspect for the hydrate research to study the affection of macroscopically kinetics conditions and the micro-mechanics in the coupling process of mechanics and chemistry to optimize the outer condition in hydrate formation process.This thesis deals with the effect of the macro kinetics parameters in the process of hydrate nucleation and growth based on the crystal nucleation theories and classic kinetics model of hydrate formation in the new spraying system, including temperature, pressure, surfactant and gas-water mixing mode, then analyzes the microcosTnic mechanism in formation process under the gas-water clusters nucleation theory proposed by Sloan E.D. in accordance with experiments. Researches show that pressure is the key factor that affects the formation of hydrate, and that under-cooling and over-pressure help to accelerate the nucleation of hydrate. Surfactant and gas-water mixing mode contribute to the enhancement of velocity of hydrate formation and reduce the energy consuming in the same time. Experiments show that the new atomization system enhances both the formation velocity and gas capacitycompared with the traditional stirring system.Under the theory of the crystal growth and with the relevant experimental data, this thesis establishes a hydrate growth mechanics- chemistry coupling calculation model in the atomization condition. Comprehensively considering the coupling mechanism of hydrate growth chemistry reaction process as well as the mechanics interactive mechanism between gas and liquid in the environment of low temperature and high pressure, the paper also thinks thoroughly about the microcosmic effects of the atomizing manners, super-saturation, mass transfer condition and different nucleation manners in the hydrate growth process. Finally, establishes a mathematically associated formula which precisely illustrates the relationship between the hydrate crystal growth and the consumption of water and gas. It is believed that the formula can be a reference to the microcosmic mechanism study of hydrate growth in the atomization condition.The thesis also makes a feasibility study for the application of hydrate technology to coal bed methane on the foundation of experiment result. An industrial process is designed for a coal bed methane well of an output ranging from 6000 to 8000m3/d with suited main facilities, meanwhile calculates the industrial energy consuming. Compared with LNG in the investment and operation expenditure, the hydrate gas storage technology has the advantage in investment, operation security and gas storage density. It will bring considerable profits to apply this technology to the exploitation of coal bed methane and the disposal of mine gas.

  • 【分类号】O621.4
  • 【下载频次】477
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