化工学报 ›› 2017, Vol. 68 ›› Issue (4): 1398-1406.DOI: 10.11949/j.issn.0438-1157.20160829

• 催化、动力学与反应器 • 上一篇    下一篇

神华上湾煤恒温阶段直接液化反应动力学

单贤根1,2, 李克健2, 章序文2, 王洪学2, 曹雪萍2, 江洪波1, 翁惠新1   

  1. 1 华东理工大学石油加工研究所, 上海 200237;
    2 中国神华煤制油化工有限公司上海研究院, 上海 201108
  • 收稿日期:2016-06-20 修回日期:2016-12-29 出版日期:2017-04-05 发布日期:2017-04-05
  • 通讯作者: 江洪波

Isothermal kinetics of direct coal liquefaction for Shenhua Shangwan coal

SHAN Xiangen1,2, LI Kejian2, ZHANG Xuwen2, WANG Hongxue2, CAO Xueping2, JIANG Hongbo1, WENG Huixin1   

  1. 1 Research Institute of Petroleum Processing, East China University of Science and Technology, Shanghai 200237, China;
    2 China Shenhua Coal to Liquid and Chemical Shanghai Research Institute, Shanghai 201108, China
  • Received:2016-06-20 Revised:2016-12-29 Online:2017-04-05 Published:2017-04-05

摘要:

为考察神华上湾煤的直接液化性能及反应动力学,以加氢蒽油-洗油混合油作为溶剂、负载型FeOOH作为催化剂,在0.01 t·d-1煤直接液化连续实验装置上考察了不同反应温度(435~465℃)、不同停留时间(7~110 min)下液化产品组成的演变规律。研究发现,随着煤的裂解及加氢反应的进行,煤及沥青类物质(PAA)收率不断减小,重质液化产物逐步向轻质液化产物转化。当反应温度为455℃、停留时间为90 min时,煤转化率为90.41%(质量分数(,油收率为61.28%(质量分数(。随着反应条件进一步苛刻,油收率下降。基于上湾煤直接液化反应特性及其产物收率变化规律建立了11集总煤直接液化反应动力学候选模型,以BFGS优化算法对实验数据搜索、选优,确定了动力学模型参数。检验结果表明所建立的动力学模型可用于恒温阶段直接液化行为的模拟计算。

关键词: 煤直接液化, 反应动力学, 集总, 模拟, 模型

Abstract:

To study the performance and reaction kinetics of direct coal liquefaction for Shenhua Shangwan coal bituminous coal, experiments were carried out in a 0.01 t·d-1 continuous tubular facility using the hydrogenated anthracene and wash oil as solvent and FeOOH as catalyst in the range of residence time 7-110 min, reaction temperature 435-465℃. The results showed that, as the coal pyrolysis and a series of hydrogenation proceed, coal and PAA yields continue to decrease, heavy liquefied product gradually transformed to light liquefied product. When the reaction temperature is 455℃, residence time of 90 min, the coal conversion reached 90.41% (mass) and oil yield 61.28% (mass) respectively, and with the reaction conditions were further harsh, the oil yield will decrease. Based on the reaction characteristics of Shenhua Shangwan coal and its data from experiments, 11 lumps reaction kinetics model was build and BFGS optimization algorithm was adopted to get reaction kinetics parameters. The kinetics model better predicted the reaction behavior of direct coal liquefaction of Shangwan coal in isothermal stage.

Key words: direct coal liquefaction, reaction kinetics, lump, simulation, model

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