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油页岩热解反应与产物优化调控研究
田勇
学位类型硕士
导师许光文 ; 高士秋  
2017-07
学位授予单位中国科学院研究生院
学位授予地点北京
学位专业化学工程
关键词油页岩 热解 调控 内构件
摘要

针对油页岩热解高收率制取高品质页岩油产品的技术需求,本论文提出通过优化调控快速热解过程的自由基生成与挥发分反应,以提高产品收率及品质的研究思路。深入研究了快速热解过程及内构件移动床调控热解产物的机理。采用两段流化床快速热解装置研究油页岩快速热解及半焦床内提质机理,探索获得高于铝甑收率、同时轻质组分(沸点低于350℃)收率高于铝甑分析油轻质组分的页岩油产品的热解条件。采用下落管耦合内构件移动床的快速热解及反应调控装置研究内构件移动床对快速热解产物的调控机理,获得下落管快速热解最佳条件,并优化内构件移动床反应温度,制取了高油收率高品质页岩油产品。本论文主要研究内容和结果如下。1、流化床快速热解及提质。单层流化床热解试验中,流化床温度在500—600℃条件下获得了高于铝甑收率的页岩油,其中在500℃下油收率最高,达到铝甑收率的1.27倍,但各温度下的热解页岩油产品中重质组分(沸点高于350℃)均超过了50%。通过将油页岩半焦添加至上部第二层流化床,使快速热解产物与半焦层接触并催化裂解,实现对重质组分的床内提质,发现双层流化床中最佳热解及提质温度为600℃,在此温度下页岩油收率下降17.74%,轻质组分收率达到7.07wt.%,上升86.11%且超过了铝甑热解的页岩油中的轻质组分收率。2、下落管快速热解耦合内构件移动床反应调控。下落管实现连续进料的油页岩颗粒快速热解,在600℃条件下获得了接近90%铝甑收率的高油收率9.59 wt.%,为优化的热解温度,在此温度下耦合了内构件移动床调控快速热解产物。实验发现,在600℃的内构件移动床温度下获得了最高油收率9.20wt%其最高轻质组分收率8.21wt.%,总收率接近铝甑收率的90%,轻质组分收率超过铝甑收油轻质组分收率的32%。内构件移动床中热解油气流经具有从高到低的温度梯度的半焦层,重质组分选择性地被吸附并催化裂解,在保留高油收率、高轻质组分含量的同时,实现重质组分截留、提质及尘过滤。确保了高油收率、高轻质组分及低尘夹带的页岩油产品。 关键词:油页岩,热解,调控,二次反应 ,内构件

其他摘要

To tackle with the technical problems in oil shale pyrolysis process to produce shale oil with high yield as well as high quality, this article puts forwards the idea of optimally controlling the process of radical generation and volatile reaction in order to promote the product yield and quality. This work deeply investigates rapid pyrolysis and the mechanism of moving bed with internals in controlling pyrolysis reaction and products. By using two-stage fluidized bed, oil shale rapid pyrolysis and in-bed oil upgrading by shale char were studied to obtain the pyrolysis condition for producing shale oil at total and light fraction (boiling point<350℃) yields higher than those of Fischer-Assay. By coupling a drop tube reactor and a moving bed with internals, their matching conditions were investigated and the optimal condition for drop tube fast pyrolysis was obtained. Shale oil product with high yield and high quality was realized. The following summarizes the main results of this study .(1)Rapid pyrolysis and upgrading characteristics in fluidized bed. Rapid pyrolysis of oil shale in one-stage fluidized bed obtained shale oil yield higher than the Fischer Assay oil yield at temperatures of 500–600 °C. The highest yield was 12.7 wt% at 500 °C and was 1.27 times of the Fischer Assay oil yield. The heavy fraction (boiling point > 350 °C) in shale oil at all temperatures of fluidized bed rapid pyrolysis was above 50%. Adding an upper fluidized bed of secondary cracking over oil shale char, found that the optimal pyrolysis and secondary cracking temperatures in such a two-stage fluidized bed were 600 °C, where the shale oil yield decreased by 17.74% but its light fraction yield was 7.07 wt% and increased by 86.11% in comparison with the light fraction yield of shale oil from the Fischer-Assay.(2) Rapid pyrolysis in a drop tube and its coupling to a moving bed with internals.Using a drop tube realized rapid pyrolysis of continuous-fed oil shale particles and the highest shale oil yield was 9.59 wt.% at 600℃, it was close to 90% of the Fischer Assay yield. Further coupling to a moving bed with internals for volatile reactions, the highest shale oil yield was 9.20wt.% at 600℃ of moving bed, which again was close to 90% of the Fischer Assay yield. Its highest light fraction yield was 8.21wt.%, above the light fraction yield from the Fischer Assay. The internals mounted in the moving bed control the pyrolysis volatile to flow in the char layer from high temperature to low temperature so that heavy fraction in volatile can be selectively adsorbed and further cracked on char particles. This process ensures the high shale oil yield and high light fraction content in oil. Meanwhile, such a flow of volatile in char bed allows dust with the volatile to be filtered to produce shale oil with low dust contamination.Key words:Oil shale, Pyrolysis, Regulation, Secondary reaction, Internals 

语种中文
文献类型学位论文
条目标识符http://ir.ipe.ac.cn/handle/122111/24213
专题研究所(批量导入)
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田勇. 油页岩热解反应与产物优化调控研究[D]. 北京. 中国科学院研究生院,2017.
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