聚磷酸铵对聚乙烯粉尘爆炸特性及热解动力学影响研究

doi:10.11949/0438-1157.20230915

化工学报 ›› 2023, Vol. 74 ›› Issue (10): 4352-4366.DOI: 10.11949/0438-1157.20230915

• 过程安全 • 上一篇

聚磷酸铵对聚乙烯粉尘爆炸特性及热解动力学影响研究

江丙友¹^,³(), 丁大伟¹^,³, 苏明清²(), 鲁昆仑¹^,³

^1.安徽理工大学工业粉尘防控与职业安全健康教育部重点实验室，安徽淮南 232001
^2.中国安全生产科学研究院，北京 100012
^3.安徽理工大学安全科学与工程学院，安徽淮南 232001

收稿日期:2023-09-01 修回日期:2023-09-24 出版日期:2023-10-25 发布日期:2023-12-22
通讯作者: 苏明清
作者简介:江丙友（1987—），男，博士，教授，cumtjiangby@163.com
基金资助:
安徽省高校杰出青年基金项目(2022AH020057);国家自然科学基金项目(52074012);安徽理工大学研究生创新基金项目(2022CX2025)

Study on the effect of ammonium polyphosphate on the explosion characteristics and pyrolysis kinetics of polyethylene dusts

Bingyou JIANG¹^,³(), Dawei DING¹^,³, Mingqing SU²(), Kunlun LU¹^,³

^1.Key Laboratory of Industrial Dust Control and Occupational Health, Ministry of Education, Anhui University of Science and Technology, Huainan 232001, Anhui, China
^2.China Academy of Safety Science and Technology, Beijing 100012, China
^3.School of Safety Science and Engineering, Anhui University of Science and Technology, Huainan 232001, Anhui, China

Received:2023-09-01 Revised:2023-09-24 Online:2023-10-25 Published:2023-12-22
Contact: Mingqing SU

摘要/Abstract

摘要：

为了减小聚乙烯（PE）粉尘爆炸事故所带来的危害，使用20-L爆炸球以及自主搭建的粉尘爆燃火焰传播测试系统进行爆炸抑制实验，从爆炸压力行为和火焰传播行为探究了聚磷酸铵（APP）对PE粉尘的抑制特性。通过同步热分析仪分析了APP对PE粉尘热解特性的影响，采用Coats-Redfern方法计算了PE和APP-PE混合粉尘（I=1.0）在快速热解阶段的反应动力学参数，并结合爆炸产物探究了其抑制机理。结果表明：APP可有效降低PE粉尘的最大爆炸压力、最大爆炸压力上升速率以及火焰传播速度，当抑制比为1.0时，PE粉尘爆炸压力峰消失，标志着在该抑制比下被完全抑制。此外，通过分析热解动力学模型发现PE粉尘在快速热解阶段遵循A3模型，添加APP后遵循R2模型，其平均活化能分别为137.34 kJ/mol和228.52 kJ/mol，活化能的增加，说明APP的加入减缓了PE粉尘的氧化和热分解，表现出显著的抑制效果。研究结果可为防治PE粉尘爆炸提供理论依据和技术支撑。

关键词: 粉体, 爆炸, 火焰传播, 聚乙烯, 聚磷酸铵, 热解特性, 动力学

Abstract:

In order to reduce the harm caused by polyethylene (PE) dust explosion accidents, a 20-L explosion ball and a self-built dust deflagration flame propagation test system were used to conduct explosion suppression experiments. The suppressive effects of ammonium polyphosphate (APP) are examined by evaluating pressure and flame propagation behavior. A synchronous thermal analyzer assesses APP’s impact on the thermal decomposition of PE dust. The reaction kinetics of PE and a mixture of APP and PE (I=1.0) during the rapid pyrolysis phase were derived employing the Coats-Redfern method. Through an in-depth analysis of explosion overpressure, flame propagation, thermal decomposition, and explosion by-products, it becomes evident that APP confers a synergistic explosion suppression effect on PE dust’s gas and condensed phases. The findings illustrate that APP markedly diminishes PE dust’s maximum explosion pressure P_max, maximum explosion pressure rate of rise (dP/dt)_max, and flame propagation speed. When the inhibition ratio was 1.0, the pressure peak vanished, indicating complete suppression of PE dust. Additionally, pyrolysis characteristics indicated that APP introduction attenuates PE dust’s pyrolysis rate and postpones pyrolysis and oxidation events. Pyrolysis kinetics model analysis showed that PE dust adheres to the A3 model during rapid pyrolysis, while it transitions to the R2 model with APP addition, with corresponding average activation energies of 137.34 kJ/mol and 228.52 kJ/mol. Significantly, APP integration results in a pronounced rise in PE’s apparent activation energy, highlighting the deceleration of PE particles’ oxidative pyrolysis. Employing FTIR analyses, a pronounced reduction in the characteristic —CH₂ and —OH peaks with APP was discerned. It’s elucidated that APP provides synergistic explosion inhibition effects in both the gas and condensed phases, primarily by curtailing free radicals via phosphorus-volatile release during pyrolysis and fostering a porous, dense surface carbon layer to inhibit deflagration. These insights lay the groundwork for the development of superior powder explosion suppressants specific to PE dust.

Key words: dust, explosion, flame propagation, polyethylene, ammonium polyphosphate, pyrolysis characteristics, kinetic

中图分类号:

X 932

江丙友, 丁大伟, 苏明清, 鲁昆仑. 聚磷酸铵对聚乙烯粉尘爆炸特性及热解动力学影响研究[J]. 化工学报, 2023, 74(10): 4352-4366.

Bingyou JIANG, Dawei DING, Mingqing SU, Kunlun LU. Study on the effect of ammonium polyphosphate on the explosion characteristics and pyrolysis kinetics of polyethylene dusts[J]. CIESC Journal, 2023, 74(10): 4352-4366.

图/表 19

表1 PE和APP物理化学性质

Table 1 Physical and chemical properties of PE and APP

样品	化学式	密度/ (g/cm³)	熔点/ ℃	分子量	D₅₀/μm
聚乙烯（PE）	(C₂H₄) _n	0.962	85	—	25.369
聚磷酸铵（APP）	(NH₄) _n₊₂P _n O₃_n₊₁	1.74	—	115	10.605

图1 APP-PE混合粉体配制实验步骤

Fig.1 Experimental steps for APP-PE hybrid powder configuration

图2 PE和APP粉尘粒径分布

Fig.2 Particle size distribution of PE and APP dust

图3 PE和APP的SEM-EDS图

Fig.3 SEM-EDS images of PE and APP

图4 20-L球形爆炸实验系统1—密封盖；2—夹层外套；3—夹层内套；4—真空表；5—循环水出口；6—气粉两相阀；7—底座；8—视窗；9—抽真空孔；10—分散阀；11—粉尘储存罐；12—压力表；13—压力传感器；14—循环水入口；15—安全限位开关；16—点火杆

Fig.4 20-L spherical explosion experimental system

图5 粉尘爆燃火焰传播测试系统1—高速摄像机；2—计算机；3—透明垂直石英玻璃管；4—点火电极；5—电磁阀；6—储气罐；7—阀门；8—压力表；9—气体管道；10—泄压阀；11—高压气瓶；12—控制系统

Fig.5 Dust deflagration flame propagation test system

图6 不同浓度PE粉尘爆炸压力曲线和爆炸特性参数变化趋势

Fig.6 Trends in explosion pressure curves and explosion characteristic parameters for different concentrations of PE dusts

图7 APP添加量对PE粉尘爆炸参数的影响

Fig.7 Effect of amount of APP on PE dust explosion parameters

图8 APP添加量对PE粉尘火焰传播的影响

Fig.8 Effect of amount of APP on PE dust flame propagation

图9 不同APP添加量下PE粉尘爆燃火焰传播前锋位置和火焰传播速度

Fig.9 PE dust deflagration flame propagation front position and flame propagation velocity under different amount of APP

表2 PE火焰灰度频数分布平均值

Table 2 Average of PE flame grey scale frequency distributions

火焰传播时间/ms	灰度均值
火焰传播时间/ms	未添加APP	0.1 g APP	0.2 g APP
60	4.2217	4.8477	1.4867
70	5.5303	5.2869	1.8246
80	7.6907	6.1680	2.0551
90	10.6845	7.7607	2.1089
95	11.9554	6.9204	2.1988
100	14.2547	10.9432	2.5561
115	22.0191	15.3787	3.9400
130	23.9056	16.3275	5.7265
140	29.0628	17.5043	9.0453
200	19.0878	15.9452	16.1389
250	9.6807	7.4677	8.7830
280	5.2990	5.6537	7.1399

图10 灰度频数分布方差

Fig.10 Variance of grey scale frequency distribution

图11 PE和APP的TG-DTG曲线分析

Fig.11 TG-DTG curve analysis of PE and APP

图12 PE与APP-PE混合粉尘(I=1.0)热解氧化动力学曲线

Fig.12 Pyrolytic oxidation kinetic curves of PE and APP-PE mixture (I=1.0)

表3 PE与APP-PE混合粉尘（I=1.0）在不同升温速率下的动力学参数

Table 3 Kinetic parameters of PE and APP-PE mixture （I=1.0） at different heating rates

样品	升温速率/ (K/min)	活化能/ (kJ/mol)	指前因子/min^-1	机理函数
PE	5	94.81	5.36×10⁵	A3模型
	10	159.17	3.95×10¹⁰	A3模型
	20	158.04	3.31×10¹⁰	A3模型
平均值		137.34	2.42×10¹⁰
APP-PE	5	224.93	6.93×10¹⁴	R2模型
	10	228.05	1.09×10¹⁵	R2模型
	20	232.59	2.60×10¹⁵	R2模型
平均值		228.52	1.46×10¹⁵

图13 实验与模拟的α-T曲线对比

Fig.13 Comparison of experimental and simulated α-T curves

图14 添加APP后PE粉尘爆炸压力特性与热解动力学的相关性

Fig.14 Correlation between explosive pressure characteristics and pyrolysis kinetics of PE dust after addition of APP

图15 添加APP前后PE粉尘爆炸残留物的傅里叶变换红外光谱a—PE爆炸前; b—PE爆炸后; c—添加抑制剂PE爆炸后

Fig.15 FTIR spectra of PE dust explosion residues before and after APP addition

图16 APP抑制PE粉尘爆炸机理分析

Fig.16 Mechanism analysis of APP inhibition of PE dust explosion

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聚磷酸铵对聚乙烯粉尘爆炸特性及热解动力学影响研究

Study on the effect of ammonium polyphosphate on the explosion characteristics and pyrolysis kinetics of polyethylene dusts

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