含氧化石墨烯NEPE推进剂在气相产物环境下的着火特性

doi:10.11949/0438-1157.20250171

摘要/Abstract

摘要：

利用快速压缩机发展了可燃混合气引燃固相推进剂的实验方法，研究了C₃H₆/O₂/Ar混合气及C₃H₆/O₂/Ar混合气+NEPE推进剂体系着火特性，使用瞬态压力传感器和高速相机同步获得了C₃H₆/O₂/Ar混合气及C₃H₆/O₂/Ar混合气+NEPE推进剂体系着火过程压力及高速图像，分析了不同C₃H₆/O₂浓度及压缩上止点压力对混合气及混合气+NEPE体系着火的影响，揭示了气相C₃H₆/O₂/Ar混合气引燃含氧化石墨烯NEPE推进剂的机制。结果表明，C₃H₆/O₂/Ar混合气的添加促进了含氧化石墨烯NEPE推进剂的着火，降低了其着火极限；随着C₃H₆/O₂浓度增加，在20 bar（1 bar=0.1 MPa）压力下，NEPE推进剂由不着火转变为着火，并在2% C₃H₆/9% O₂/89% Ar混合气（Mix3）条件下发生爆燃；随着压缩上止点压力的增加，Mix4与Mix4+NEPE体系由不着火转变为着火，且着火延迟期逐渐缩短。

关键词: NEPE推进剂, 丙烯, 快速压缩机, 着火延迟期, 爆燃

Abstract:

An experimental method for igniting solid propellants with combustible gas mixture was developed using a rapid compression machine (RCM), and the ignition characteristics of C₃H₆/O₂/Ar mixture and C₃H₆/O₂/Ar mixture + NEPE propellant system were studied. Transient pressure sensors and high-speed camera were employed to simultaneously obtain the pressure and high-speed images of the ignition process for both the C₃H₆/O₂/Ar gas mixture and the C₃H₆/O₂/Ar gas mixture + NEPE propellant system. The effects of different C₃H₆/O₂ concentrations and pressures on the ignition of the gas mixture and the gas mixture + NEPE system were analyzed. The mechanism of the gaseous C₃H₆/O₂/Ar mixture igniting NEPE propellant was revealed. The results show that the addition of C₃H₆/O₂/Ar gas mixture promotes the ignition of NEPE propellant containing graphene oxide and lowers its ignition limit. As the concentration of C₃H₆/O₂increases, at a pressure of 20 bar, the NEPE propellant transitions from non-ignition to ignition, and a deflagration occurs under the condition of a 2% C₃H₆/9% O₂/89% Ar gas mixture (Mix3). With the increase of pressure, both the Mix4 and Mix4 + NEPE propellant systems transition from non-ignition to ignition, and the ignition delay time gradually shortens.

Key words: NEPE propellant, propylene, rapid compression machine, ignition delay time, deflagration

中图分类号:

V 512

杨猛, 嵇宣哲, 刘畅, 余涛, 付小龙, 黄佐华, 汤成龙. 含氧化石墨烯NEPE推进剂在气相产物环境下的着火特性[J]. 化工学报, 2025, 76(9): 4893-4902.

Meng YANG, Xuanzhe JI, Chang LIU, Tao YU, Xiaolong FU, Zuohua HUANG, Chenglong TANG. Ignition characteristics of NEPE propellant containing graphene oxide in gaseous product environment[J]. CIESC Journal, 2025, 76(9): 4893-4902.

图/表 12

表1 测试工况和反应物组分

Table 1 Test conditions and reactant mixtures

Mix	体积分数/%			p_c/bar
Mix	C₃H₆	O₂	Ar	p_c/bar
1	0.5	2.25	97.25	20、25、30、35
2	1	4.5	94.5	20、25、30、35
3	2	9	89	20、25、30、35
4	1	2.25	96.75	20、25、30、35

图1 快速压缩机装置

Fig.1 The schematic of the rapid compression machine

图2 RCM典型的压力曲线以及IDT定义

Fig.2 Typical pressure trace and IDT definition of the RCM

图3 Mix1/Mix1+NEPE体系在20 bar、1042 K下的压力曲线

Fig.3 Pressure traces of Mix1/Mix1+NEPE system at 20 bar and 1042 K

图4 Mix1/Mix1+NEPE体系在20 bar、1042 K下的高速图像

Fig.4 High-speed imgaes of Mix1/Mix1+NEPE system at 20 bar and 1042 K

图5 Mix2/Mix2+NEPE体系在20 bar、993.2 K下的压力曲线

Fig.5 Pressure traces of Mix2/Mix2+NEPE system at 20 bar and 993.2 K

图6 Mix2/Mix2+NEPE体系在20 bar、993.2 K下的高速图像

Fig.6 High-speed images of Mix2/Mix2+NEPE system at 20 bar and 993.2 K

图7 Mix3/Mix3+NEPE体系在20 bar、895.1 K下的压力曲线

Fig.7 Pressure traces of Mix3/Mix3+NEPE system at 20 bar and 895.1 K

图8 Mix3/Mix3+NEPE体系在20 bar、895.1 K下的高速图像

Fig.8 High-speed images of Mix3/Mix3+NEPE system at 20 bar and 895.1 K

图9 不同压力下Mix4与Mix4+NEPE体系的着火压力曲线

Fig.9 Pressure traces of Mix4 and Mix4+NEPE systems at different pressures

图10 Mix4/Mix4+NEPE体系在30 bar、980 K下的高速图像

Fig.10 High-speed images of Mix4/Mix4+NEPE system at 30 bar and 980 K

表2 不同混合气及混合气+NEPE体系在不同压力下的着火情况

Table 2 Ignition behaviors of different Mix and Mix+NEPE systems at different pressures

T	混合气	着火情况
T	混合气	20 bar	25 bar	30 bar	35 bar
1040 K	Mix1	×	×	×	√
1040 K	Mix1+NEPE	√	√	√	√
995 K	Mix2	√	√	√	√
995 K	Mix2+NEPE	√	√	√	√
895 K	Mix3	√	√	√	√
895 K	Mix3+NEPE	√√	√√	√√	√√
980 K	Mix4	×	×	×	√
980 K	Mix4+NEPE	×	×	√	√

参考文献 30

[1]	Wang Y L, Rong H, Zhang X H, et al. Influences of Bu-NENA and BDNPA/F plasticizers on the properties of binder for high-energy NEPE propellants[J]. Propellants, Explosives, Pyrotechnics, 2021, 46(6): 950-961.
[2]	刘瀚文, 付小龙, 王江宁, 等. 基于近场动力学方法的NEPE推进剂断裂失效研究[J]. 兵工学报, 2024.
	Liu H W, Fu X L, Wang J N, et al. Study on fracture failure of NEPE propellant based on near-field dynamics method[J]. China Industrial Economics, 2024.
[3]	Li H, Xu J S, Chen X, et al. Experimental investigation and modeling the compressive behavior of NEPE propellant under confining pressure[J]. Propellants, Explosives, Pyrotechnics, 2021, 46(7): 1023-1035.
[4]	李世奇, 强洪夫, 陈铁铸, 等. 单轴拉伸下NEPE固体推进剂细观结构演化行为研究[J]. 含能材料, 2024, 32(2): 175-182.
	Li S Q, Qiang H F, Chen T Z, et al. Mesostructure evolution behavior of NEPE solid propellant under uniaxial tension[J]. Chinese Journal of Energetic Materials, 2024, 32(2): 175-182.
[5]	Yang M, Yu T, Meng S Q, et al. Effects of graphene oxide addition on ignition sensitivity and burning rate of NEPE propellant under rapid thermal stimulus[J]. Combustion and Flame, 2024, 266: 113500.
[6]	杨猛, 方鸣, 余涛, 等. 氧化石墨烯对含CL-20的NEPE推进剂热分解及燃烧性能的影响[J]. 推进技术, 2025, 46(3): 188-195.
	Yang M, Fang M, Yu T, et al. Effects of graphene oxide on thermal decomposition and combustion performance of NEPE propellant containing CL-20[J]. Journal of Propulsion Technology, 2025, 46(3): 188-195.
[7]	王芳, 张小平, 胡润芝, 等. 硝酸酯增塑聚醚高能推进剂高压燃烧性能研究[J]. 推进技术, 2004, 25(5): 469-472.
	Wang F, Zhang X P, Hu R Z, et al. Study on combustion properties of nitrate ester plasticized polyether propellants at high pressure[J]. Journal of Propulsion Technology, 2004, 25(5): 469-472.
[8]	Sha B S, Na X D, Xia Z X, et al. Experimental study on the combustion characteristics of aluminized nitrate ester plasticized polyether solid propellant under high pressure[J]. Acta Astronautica, 2022, 193: 100-109.
[9]	涂乘崟, 庄宇倩, 李映坤, 等. NEPE推进剂燃烧过程及铝团聚特性[J]. 航空动力学报, 2023, 38(11): 2791-2798.
	Tu C Y, Zhuang Y Q, Li Y K, et al. Combustion process and aluminum agglomeration characteristics of NEPE propellant[J]. Journal of Aerospace Power, 2023, 38(11): 2791-2798.
[10]	涂乘崟, 凌志刚, 董龙龙, 等. NEPE推进剂燃烧表面铝团聚物动态行为研究[J]. 推进技术, 2023, 44(3): 248-256.
	Tu C Y, Ling Z G, Dong L L, et al. Dynamic behavior study of aluminum aggregates on NEPE propellant combustion surface[J]. Journal of Propulsion Technology, 2023, 44(3): 248-256.
[11]	Tu C Y, Feng Y Y, Ling Z G, et al. Thermal decomposition, ignition process and combustion behavior of nitrate ester plasticized polyether propellant at 0.1—3.0 MPa[J]. International Journal of Aerospace Engineering, 2022, 2022(1): 6439787.
[12]	李疏芬, 牛和林, 张钢锤, 等. NEPE推进剂激光点火特性[J]. 推进技术, 2002, 23(2): 172-175.
	Li S F, Niu H L, Zhang G C, et al. Laser ignition of NEPE propellant[J]. Journal of Propulsion Technology, 2002, 23(2): 172-175.
[13]	Yan X T, Xia Z X, Huang L Y, et al. Combustion of nitrate ester plasticized polyether propellants[J]. Journal of Zhejiang University Science A, 2020, 21(10): 834-847.
[14]	相恒升, 陈雄, 周长省, 等. 环境气体氧含量对NEPE推进剂激光点火过程的影响[J]. 火炸药学报, 2016, 39(3): 75-79.
	Xiang H S, Chen X, Zhou C S, et al. Effect of oxygen content in environment gas on the laser ignition process of NEPE propellant[J]. Chinese Journal of Explosives & Propellants, 2016, 39(3): 75-79.
[15]	涂乘崟, 陈雄, 周长省, 等. NEPE推进剂在氮气及空气中的点火燃烧特性[J]. 含能材料, 2022, 30(8): 811-818.
	Tu C Y, Chen X, Zhou C S, et al. Ignition and combustion characteristics of NEPE propellant in nitrogen and air[J]. Chinese Journal of Energetic Materials, 2022, 30(8): 811-818.
[16]	Yan Q L, Liu P J, He A F, et al. Photosensitive but mechanically insensitive graphene oxide-carbohydrazide-metal hybrid crystalline energetic nanomaterials[J]. Chemical Engineering Journal, 2018, 338: 240-247.
[17]	王帅中, 王健, 张嘉玲, 等. 氧化石墨烯基含能配位聚合物对四组元复合推进剂热分解及燃烧催化作用[J]. 火炸药学报, 2021, 44(3): 308-315.
	Wang S Z, Wang J, Zhang J L, et al. Catalytic effect of graphene oxide based energetic coordination polymers on thermal decomposition and combustion behavior of four-component composite propellant[J]. Chinese Journal of Explosives & Propellants, 2021, 44(3): 308-315.
[18]	Memon N K, McBain A W, Son S F. Graphene oxide/ammonium perchlorate composite material for use in solid propellants[J]. Journal of Propulsion and Power, 2016, 32(3): 682-686.
[19]	Zhang X, Hikal W M, Zhang Y, et al. Direct laser initiation and improved thermal stability of nitrocellulose/graphene oxide nanocomposites[J]. Applied Physics Letters, 2013, 102(14): 141905.
[20]	Ye B Y, An C W, Zhang Y R, et al. One-step ball milling preparation of nanoscale CL-20/graphene oxide for significantly reduced particle size and sensitivity[J]. Nanoscale Research Letters, 2018, 13(1): 42.
[21]	Li R, Wang J, Shen J P, et al. Preparation and characterization of insensitive HMX/graphene oxide composites[J]. Propellants, Explosives, Pyrotechnics, 2013, 38: 798-804.
[22]	杨猛, 丁晓倩, 余涛, 等. 甲烷/氧化亚氮绿色推进剂自着火特性实验及动力学[J]. 化工学报, 2025, 76(3): 1221-1229.
	Yang M, Ding X Q, Yu T, et al. Experimental and kinetic studies for the ignition characteristic of the green propellant of methane/nitrous oxide[J]. CIESC Journal, 2025, 76(3): 1221-1229.
[23]	Yang M, Liao C Y, Tang C L, et al. The auto-ignition behaviors and risk assessments of double-base propellant containing different 1,1-diamino-2,2-dinitroethene particle sizes under rapid heating[J]. Combustion and Flame, 2021, 234: 111627.
[24]	Yang M, Wu Y T, Tang C L, et al. Auto-ignition behaviors of nitromethane in diluted oxygen in a rapid compression machine: critical conditions for ignition, ignition delay times measurements, and kinetic modeling interpretation[J]. Journal of Hazardous Materials, 2019, 377: 52-61.
[25]	Yang M, Liao C Y, Tang C L, et al. The auto-ignition behaviors of HMX/NC/NG stimulated by heating in a rapid compression machine[J]. Fuel, 2021, 288: 119693.
[26]	Yang M, Ma X, Huang Z H, et al. Role of O₂ on nitrous oxide fuel blend ethylene auto-ignition sensitivity[J]. Combustion and Flame, 2024, 259: 113167.
[27]	Mittal G, Sung C J. A rapid compression machine for chemical kinetics studies at elevated pressures and temperatures[J]. Combustion Science and Technology, 2007, 179(3): 497-530.
[28]	Goldsborough S S, Hochgreb S, Vanhove G, et al. Advances in rapid compression machine studies of low-and intermediate-temperature autoignition phenomena[J]. Progress in Energy and Combustion Science, 2017, 63: 1-78.
[29]	Wu Y T, Yang M, Tang C L, et al. Promoting “adiabatic core” approximation in a rapid compression machine by an optimized creviced piston design[J]. Fuel, 2019, 251: 328-340.
[30]	Di H S, He X, Zhang P, et al. Effects of buffer gas composition on low temperature ignition of iso-octane and n-heptane [J]. Combustion and Flame, 2014, 161(10): 2531-2538.