高压聚乙烯失控分解研究进展：反应机理、引发体系与模型

doi:10.16085/j.issn.1000-6613.2023-0739

化工进展 ›› 2023, Vol. 42 ›› Issue (8): 3979-3989.DOI: 10.16085/j.issn.1000-6613.2023-0739

高压聚乙烯失控分解研究进展：反应机理、引发体系与模型

张智琛¹(), 朱云峰¹, 成卫戍², 马守涛¹, 姜杰¹, 孙冰¹(), 周子辰², 徐伟¹()

^1.化学品安全全国重点实验室，中石化安全工程研究院有限公司，应急管理部化学品登记中心，山东青岛 266000
^2.中国石油化工股份有限公司北京燕山分公司，北京 102500

收稿日期:2023-05-06 修回日期:2023-06-14 出版日期:2023-08-15 发布日期:2023-09-19
通讯作者: 孙冰,徐伟
作者简介:张智琛（1993—），男，工程师，研究方向为化工过程安全。E-mail：zhangzc.qday@sinopec.com。
基金资助:
国家自然科学基金(22278452)

Research advances on runaway decomposition of high pressure polyethylene: Reaction mechanism, initiation system and model

ZHANG Zhichen¹(), ZHU Yunfeng¹, CHENG Weishu², MA Shoutao¹, JIANG Jie¹, SUN Bing¹(), ZHOU Zichen², XU Wei¹()

^1.State Key Laboratory of Chemical Safety, SINOPEC Research Institute of Safety Engineering Co. , Ltd. , National Registration Center for Chemicals, Ministry of Emergency Management, Qingdao 266000, Shandong, China
^2.SINOPEC Yanshan Petrochemical Company, Beijing 102500, China

Received:2023-05-06 Revised:2023-06-14 Online:2023-08-15 Published:2023-09-19
Contact: SUN Bing, XU Wei

摘要/Abstract

摘要：

高压聚乙烯又名低密度聚乙烯（LDPE），是当前世界上用途广泛和产量较大的塑料制品。然而LDPE的合成需要在高于150MPa的工艺条件下进行，燃爆风险高。本文对LDPE高压聚合工艺过程进行了介绍，探讨了LDPE合成过程中的聚合与分解机理，分析了引发剂和高温热点导致乙烯失控分解的致灾机制，对聚合条件下乙烯失控分解的关键参数和极限边界进行了阐述。此外，对乙烯分解的数学模型及发展进行了介绍和论述。最后，本文提出了当前应对LDPE本质安全化生产所需解决的问题，并对此提出了解决思路与发展方向，以期为我国自主知识产权的LDPE工艺安全发展提升提供思考。

关键词: 高压聚乙烯, 乙烯, 引发剂, 失控分解, 模型

Abstract:

High pressure polyethylene, as known as low density polyethylene (LDPE), is the most widely used plastic products in the world. However, LDPE preparation needs to be carried out under high pressure process, and then ethylene will decompose out of control under adiabatic compression condition with a large risk of ignition and explosion. This paper analyzed the causes of LDPE production accidents at home and abroad in recent years, introduced the high pressure polymerization process of LDPE and discussed the polymerization and decomposition mechanism of LDPE synthesis in detail. The main causes of the runaway decomposition of ethylene caused by initiators and hot spots at high temperature were summarized, and the key parameters as well as limit boundary of the runaway decomposition of ethylene under polymerization conditions were also described carefully. In addition, the mathematical model and development of ethylene decomposition were fully introduced and discussed. Finally, this paper put forward the problems that needed to be solved to deal with the essential safety production of LDPE, and proposed the solution and future development direction to provide thinking for the future safety development of LDPE process and capacity improvement.

Key words: high pressure polyethylene, ethylene, initiator, runaway decomposition, model

中图分类号:

TQ32

张智琛, 朱云峰, 成卫戍, 马守涛, 姜杰, 孙冰, 周子辰, 徐伟. 高压聚乙烯失控分解研究进展：反应机理、引发体系与模型[J]. 化工进展, 2023, 42(8): 3979-3989.

ZHANG Zhichen, ZHU Yunfeng, CHENG Weishu, MA Shoutao, JIANG Jie, SUN Bing, ZHOU Zichen, XU Wei. Research advances on runaway decomposition of high pressure polyethylene: Reaction mechanism, initiation system and model[J]. Chemical Industry and Engineering Progress, 2023, 42(8): 3979-3989.

图/表 12

图1 LDPE装置工艺流程[6]

表1 LDPE生产中常用的有机过氧化物

项目	化学名称	半衰期为1min时的温度/℃
低温系列	过氧化二碳酸二-2-乙基己酯	91
	过氧癸酸叔丁酯	101
	过氧化十二酰	113
	过氧新戊酸叔丁酯	110
	过氧化异丁酰	113
	过氧化-2-乙基氧甲酸叔丁酯	135
中温系列	叔丁基过氧异丙基碳酸酯	158
	叔丁基过氧乙酸	160
	过氧苯甲酸叔丁酯	170
高温系列	二叔丁基过氧化物	186
	1,1,3,3-四甲基丁基过氧化氢	223

图2 沿LDPE管式反应器长度的环境示意图[55]

图3 环境1内不同单体进料温度、体积分数和入口引发剂浓度的局部失控边界预测

图4 乙酸乙烯对乙烯热失控和热点触发分解边界的影响关系图（图中百分数均为质量分数）

图5 LDPE聚合过程中分解的压力和温度过程

图6 纯乙烯与乙烯-乙酸乙烯混合物的分解边界

图7 乙烯-质量分数10%乙酸乙烯体系的最大爆炸压力与初始压力和壁温的关系

图8 最大爆炸压力与单体混合物密度的函数关系

图9 乙烯-质量分数10%乙酸乙烯体系的最大压力增加速率随初始压力和壁温变化图

图10 热失控后气态分解产物

图11 乙酸乙烯对乙烯分解边界的影响

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高压聚乙烯失控分解研究进展：反应机理、引发体系与模型

Research advances on runaway decomposition of high pressure polyethylene: Reaction mechanism, initiation system and model

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