【摘要】：加強瓦斯水合反應的熱量、物質傳遞過程,有效控制水合反應速率、提高水合物產(chǎn)量是實現(xiàn)瓦斯水合固化儲運技術工業(yè)化應用的關鍵。因此,本文在諸多國內(nèi)外科研工作學者研究基礎上,針對甲烷含量為60%、70%、80%的高濃度瓦斯混合氣,分別開展純水靜態(tài)(空白)體系和機械噴霧強化體系水合反應實驗,考察機械噴霧手段、霧化噴嘴夾角、噴嘴流量對瓦斯水合物生長速率、CH4回收率、分離因子和分配系數(shù)的影響并基于傳熱-傳質理論模型初步分析了影響機理。純水靜態(tài)體系和機械噴霧體系實驗結果對比表明:瓦斯混合氣樣G1、G2、G3在機械噴霧強化體系下的水合分離效果都優(yōu)于純水靜態(tài)體系,其對應的水合物生長速率最大值分別為0.395×10-6、0.379×10-6、0.367×10-6m3/min,相比純水靜態(tài)體系分別提高了5.41、2.63、3.71倍;CH4回收率最大值分別為24.23%、25.27%、24.51%,相比純水靜態(tài)體系分別提高了6.18、2.61、7.19倍;分離因子最大值分別為1.89、1.83、1.95,相比純水靜態(tài)體系分別提高了1.62、1.49、1.74倍;分配系數(shù)最大值分別為1.27、1.19、1.13,相比純水靜態(tài)體系分別提高了1.2、1.12、1.11倍。綜上所述,在三種瓦斯氣樣都采用機械噴霧手段強化水合分離過程的狀況下,對比相應的純水靜態(tài)體系,氣樣G1在水合物生長速率、分配系數(shù)方面改善幅度最大;氣樣G3在CH4回收率、分離因子方面改善幅度最大。不同霧化噴嘴夾角實驗結果對比表明:相同驅動力、噴嘴流量實驗條件下,瓦斯混合氣樣G1、G2、G3的水合物生長速率、CH4回收率、分離因子和分配系數(shù)受霧化噴嘴夾角影響規(guī)律一致,都是隨夾角度數(shù)的升高先增大后減小,影響順序為:45°30°60°90°。分析認為,30°、45°霧化噴嘴對反應體系水合物生長環(huán)境影響較小,60°、90°霧化噴嘴對反應體系水合物生長環(huán)境影響較為惡劣。不同噴嘴流量實驗結果對比表明:相同驅動力、霧化噴嘴夾角實驗條件下,瓦斯混合氣樣G1、G2、G3的水合物生長速率、CH4回收率、分離因子和分配系數(shù)受噴嘴流量影響規(guī)律也一致,流量為20ml/min的噴嘴對反應體系水合分離促進效果優(yōu)于流量為10ml/min的噴嘴。分析認為,增大噴霧循環(huán)體系噴嘴流量,不僅能夠加強氣液間的物質(分子)傳遞過程,也能加快反應體系水合物生成熱的流失速率。本文研究成果對后續(xù)相關研究工作的實驗開展與水合物工業(yè)生產(chǎn)具有重要科學意義與指導價值。
[Abstract]:The key to realize the industrial application of gas hydration curing storage and transportation technology is to strengthen the heat transfer process of gas hydration reaction effectively control the hydration reaction rate and increase the hydrate production. Therefore, based on the research of many domestic and foreign researchers, the hydration experiments of pure water static (blank) system and mechanical spray strengthened system were carried out for the high concentration gas mixture with methane content of 60% or 70%. The effects of mechanical spray method, atomizing nozzle angle, nozzle flow rate on methane hydrate growth rate and CH4 recovery, separation factor and distribution coefficient were investigated. Based on the heat and mass transfer theory model, the influence mechanism was preliminarily analyzed. The experimental results of pure water static system and mechanical spray system show that the hydration separation effect of gas mixture G1G2G3 is better than that of pure water static system. The maximum rate of hydrate growth was 0.395 脳 10-6 (0.379 脳 10-6) 0.367 脳 10-6m3 / min, respectively. Compared with the pure water static system, the maximum recovery rate of CH4 was increased by 5.41 ~ 2.63 ~ 3.71 times, respectively, and the maximum recovery rate of Ch _ 4 was 24.23 ~ 25.27 ~ 24.51% and 6.18 ~ 2.61g ~ (7.19) times higher than that of pure water static system, respectively. The maximum value of separation factor was 1.89 ~ 1.83 ~ 1.95, which was 1.62 ~ 1.49 ~ 1.74 times higher than that of pure water static system, and the maximum partition coefficient was 1.27 ~ 1.19 ~ 1.13, 1.22 ~ 1.12 ~ 1.11 times higher than that of pure water static system, respectively. In conclusion, under the condition that all three kinds of gas samples strengthen hydration separation process by mechanical spray, compared with the corresponding pure water static system, the gas sample G1 has the greatest improvement in hydrate growth rate and distribution coefficient. Gas sample G 3 has the greatest improvement in CH4 recovery and separation factor. The experimental results of different atomization nozzle angles show that under the same driving force and nozzle flow test conditions, the gas mixture G1G2G3 hydrate growth rate and CH4 recovery rate, separation factor and distribution coefficient are consistent with the influence of atomizing nozzle angle on gas hydrate growth rate. The influence order is 45 擄30 擄60 擄90 擄. It is considered that the influence of 30 擄~ 45 擄atomization nozzle on the hydrate growth environment of the reaction system is less than that of the 60 擄~ 90 擄atomizing nozzle on the reaction system hydrate growth environment. The experimental results of different nozzles showed that under the same driving force and atomization nozzle angle, the gas mixture G1G2G3 hydrate growth rate and CH4 recovery rate, separation factor and distribution coefficient influenced by nozzle flow rate were also consistent. The effect of the nozzle with flow rate of 20ml/min on the hydration separation of reaction system is better than that of the nozzle with flow rate of 10ml/min. It is concluded that increasing the nozzle flow rate of the spray cycle system can not only enhance the material (molecular) transfer process between gas and liquid, but also accelerate the heat loss rate of hydrate formation in the reaction system. The research results in this paper are of great scientific significance and guiding value for the experimental development of related research work and the production of hydrate industry.
【學位授予單位】：黑龍江科技大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：TD712

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