甲烷和环辛烷sH水合物的热力学、动力学、形态和拉曼光谱研究

IF 4.3 Q2 ENGINEERING, CHEMICAL ACS Engineering Au Pub Date : 2023-02-06 DOI:10.1021/acsengineeringau.2c00050
Namrata Gaikwad, Hyunho Kim, Gaurav Bhattacharjee, Jitendra S Sangwai, Rajnish Kumar* and Praveen Linga*, 
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引用次数: 1

摘要

在不久的将来,天然气有望成为主要的能源来源,而以天然气水合物的形式储存天然气是一种安全、清洁、经济的方法。然而,所需的热力学条件和慢动力学是工艺可行性需要解决的关键挑战。本研究包括利用热力学、动力学、形态学和拉曼分析对甲烷和环辛烷sH水合物形成的可能应用进行实验研究。水合物的形成是在只形成sH水合物的热力学条件下进行的。通过相边界解离法研究甲烷和环辛烷体系的四相(Lw-LHC-H-V) sH水合物平衡,该方法是一种可靠的方法,因为与其他可用方法相比,它在单次实验运行中提供了更多的平衡数据点。与sI水合物形成相比,sH水合物的形成有助于降低平衡条件。使用低色氨酸浓度可以改善sH水合物的缓慢形成动力学。在这项工作中,0.1 wt %的色氨酸浓度是气体吸收的最佳浓度,与0.01、0.05和1 wt %的色氨酸浓度相比,水合物形成率最高。在这里,我们也从视觉上研究了sH水合物的形成,并观察到在没有色氨酸的系统中,水合物的形成发生在界面以下;然而,随着色氨酸浓度的增加,界面上方的水合物形成增加。水合物形成的增加可能是由于水合物形成的多孔性日益增加而增加的气体吸收量。拉曼分析证实了水合物笼中甲烷和环辛烷的存在。与不使用色氨酸的体系相比,使用色氨酸的峰强度更高,进一步证实了更高的水合物形成。
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Thermodynamics, Kinetics, Morphology, and Raman studies for sH Hydrate of Methane and Cyclooctane

Natural gas is expected to be the major energy source in the near future, and storing it in the form of gas hydrate is a safe, clean, and economical approach. However, required thermodynamic conditions and slow kinetics are the key challenges that need to address for process viability. This study involves an experimental investigation of methane and cyclooctane sH hydrate formation for possible applications in gas storage using thermodynamics, kinetics, morphology, and Raman analysis. The hydrate formation is carried out at such thermodynamic conditions where only sH hydrate would form. The four-phase (Lw-LHC-H-V) sH hydrate equilibrium is studied for the methane and cyclooctane system via dissociation along the phase boundary method which is a robust method as it delivers a greater number of equilibrium data points in a single experimental run compared to other available methods. The sH hydrate formation helps in lowering the equilibrium conditions compared with sI hydrate formation. The slow sH hydrate formation kinetics can be improved by using low tryptophan concentrations. In this work, 0.1 wt % is the optimum tryptophan concentration as the gas uptake, and the hydrate formation rate is found to be the highest compared to 0.01, 0.05, and 1 wt % tryptophan concentrations. Here, we also visually investigate the sH hydrate formation and observed that the hydrate formation occurs below the interface for the system with no tryptophan; however, hydrate formation occurrence above the interface increases with an increase in the tryptophan concentration. The increase in the hydrate formation could be dedicated to the increased gas uptake due to the increasingly porous nature of hydrate formation. The Raman analysis confirmed the presence of methane and cyclooctane in sH hydrate cages. The higher intensity of the peaks using tryptophan additionally confirms the higher hydrate formation compared to the system with no tryptophan.

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ACS Engineering Au
ACS Engineering Au 化学工程技术-
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期刊介绍: )ACS Engineering Au is an open access journal that reports significant advances in chemical engineering applied chemistry and energy covering fundamentals processes and products. The journal's broad scope includes experimental theoretical mathematical computational chemical and physical research from academic and industrial settings. Short letters comprehensive articles reviews and perspectives are welcome on topics that include:Fundamental research in such areas as thermodynamics transport phenomena (flow mixing mass & heat transfer) chemical reaction kinetics and engineering catalysis separations interfacial phenomena and materialsProcess design development and intensification (e.g. process technologies for chemicals and materials synthesis and design methods process intensification multiphase reactors scale-up systems analysis process control data correlation schemes modeling machine learning Artificial Intelligence)Product research and development involving chemical and engineering aspects (e.g. catalysts plastics elastomers fibers adhesives coatings paper membranes lubricants ceramics aerosols fluidic devices intensified process equipment)Energy and fuels (e.g. pre-treatment processing and utilization of renewable energy resources; processing and utilization of fuels; properties and structure or molecular composition of both raw fuels and refined products; fuel cells hydrogen batteries; photochemical fuel and energy production; decarbonization; electrification; microwave; cavitation)Measurement techniques computational models and data on thermo-physical thermodynamic and transport properties of materials and phase equilibrium behaviorNew methods models and tools (e.g. real-time data analytics multi-scale models physics informed machine learning models machine learning enhanced physics-based models soft sensors high-performance computing)
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