Spray flash evaporation preparation of micro/nanoparticles

doi:10.11949/0438-1157.20240811

Abstract

Abstract:

This study presents the design and construction of an experimental device for the preparation of micro/nanoparticles through a spray flash evaporation. Solutions containing organic solutes are sprayed into a vacuum flash evaporation chamber to obtain the organic micro/nanoparticles. The experiment included an initial pressure of 3.0—4.5 MPa, an initial temperature of 130—200℃, three sets of nozzles with different diameters, and four sets of organic solutes. Using the 0.10 mm nozzle, the particle size distribution of p-toluene sulfonamide ranges from 0 to 30 μm. When the initial conditions are increased to 4.5 MPa and 170℃, the proportion of particles smaller than 6 μm can be increased to 62% and 75%, respectively. This indicates that increasing the initial conditions has a significant refinement effect on the particles. In addition, increasing the nozzle size will further increase the particle size and non-uniformity due to the suppression of flash evaporation caused by the deterioration of atomization effect. Therefore, the small diameter nozzle can produce smaller, more concentrated, and uniformly distributed micro/nanoparticles. The particle morphology and size of different organic solutes are different, but the particle size is distributed within 40 μm, indicating that this experimental device has a certain universality.

Key words: spray flash evaporation, organic solutes, preparation, micro/nanoparticles, particle formation, particle size distribution

摘要：

设计并搭建了一套通过喷雾闪蒸方法制备微纳米颗粒的实验装置，将含有有机溶质的溶液喷入真空腔室内进行闪蒸，以得到相应的微纳米有机颗粒。实验涵盖了3.0~4.5 MPa的初始压力、130~200℃的初始温度以及三组不同直径的喷嘴和四种有机物溶质。使用0.10 mm的喷嘴，制得的对甲苯磺酰胺颗粒尺寸分布在0~30 μm。提高喷雾初始温度与压力可使小尺寸颗粒占比提高，平均直径减小，这对颗粒的细化作用十分明显。当增大喷嘴直径时，雾化效果变差对闪蒸的抑制将会增大颗粒的尺寸和不均匀性，因此使用小口径喷嘴能够获得更小、分布更集中的颗粒。而不同有机溶质制得的颗粒形态与大小均有不同，但颗粒尺寸都分布在40 μm以内，表明本实验装置具有一定的普适性。

关键词: 喷雾闪蒸, 有机溶质, 制备, 微纳米颗粒, 粒子形成, 粒度分布

CLC Number:

TK 124

Ben’an CAI, Jianxin ZHANG, Chengjun LONG, Qiaochen DU, Xunjian CHE, Yiying ZHANG, Weihua CAI. Spray flash evaporation preparation of micro/nanoparticles[J]. CIESC Journal, 2025, 76(3): 1334-1345.

蔡本安, 张建新, 龙城君, 杜乔琛, 车勋建, 张义迎, 蔡伟华. 喷雾闪蒸制备微纳米颗粒[J]. 化工学报, 2025, 76(3): 1334-1345.

Figures/Tables 16

Table 1 Experimental reagents

药品名称	化学式	纯度	厂家
乙醇	C₂H₆O	>99%	三合酒精
对甲苯磺酰胺	C₇H₉NO₂S	GR，>99%	麦克林
丁二酸	C₄H₆O₄	AR，>99%	科密欧
苹果酸	C₂H₆O₅	AR，>99%	福晨
葡萄糖	C₆H₁₂O₆	GR，>99%	科密欧

Fig.1 Schematic diagram of experimental system

Table 2 Selection of experimental parameters

参数	选取范围
初始温度/℃	130~200
初始压力/MPa	3.0~4.5
喷嘴尺寸/mm	0.10、0.15、0.20
闪蒸罐真空压力/Pa	2000~3000
喷射方向	竖直向下

Table 3 Uncertainty of experimental instruments

实验仪器	精确性	测试范围	不确定度
压力变送器	±0.5%	0~5000 Pa	±1.52%
压力变送器	±0.5%	0~8 MPa	±1.36%
流量计	±0.5%	1~18 L/h	±1.3%
热电偶	±1%	0~600℃	±1%

Fig.2 The shape of the spray under different initial pressures

Fig.3 The shape of the spray under different nozzle sizes

Fig.4 The SEM images of p-toluene sulfonamide at different initial temperatures

Fig.5 Particle size distribution at different initial temperatures

Fig.6 The variation of particle diameter with initial temperature and Ja

Fig.7 SEM images of p-toluene sulfonamide at different initial pressures

Fig.8 Particle size distribution at different initial pressures

Fig.9 Average particle size varies with the initial pressure

Fig.10 SEM images of p-toluene sulfonamide at different nozzle diameters

Fig.11 Particle size distribution under different nozzle diameters

Fig.12 SEM images of particles obtained from different organic solutes

Fig.13 Particle size distribution obtained from different organic solutes

References 31

1	陈成克, 姜从强, 蒋梅燕, 等. 石墨基底上制备TaC纳米颗粒的研究[J]. 浙江工业大学学报, 2022, 50(6): 671-678.
	Chen C K, Jiang C Q, Jiang M Y, et al. Study on the preparation of TaC nanoparticles on graphite substrate[J]. Journal of Zhejiang University of Technology, 2022, 50(6): 671-678.
2	房迅, 王嘉伟, 吴迎花, 等. 银纳米颗粒的制备、抑菌机制及应用的研究进展[J]. 化工技术与开发, 2023, 52(8): 33-37.
	Fang X, Wang J W, Wu Y H, et al. Progress of preparation, bacteriostatic mechanism and application of silver nanoparticles[J]. Technology & Development of Chemical Industry, 2023, 52(8): 33-37.
3	张明珠, 于涛. 羟基喜树碱纳米微米制剂研究进展[J]. 现代农业科技, 2016(1): 227-228, 230.
	Zhang M Z, Yu T. Research advances on hydroxycamptothecin nano and micro formulations[J]. Modern Agricultural Science and Technology, 2016(1): 227-228, 230.
4	刘春华, 杨秀培, 吴莉宇, 等. 纳米银胶体粒子的制备及对牛血清蛋白的检测[J]. 化学研究与应用, 2008, 20(6): 786-789.
	Liu C H, Yang X P, Wu L Y, et al. Preparation of nano-silver colloid and its application on quantitative analysis of BSA[J]. Chemical Research and Application, 2008, 20(6): 786-789.
5	Yao R S, Liu L, Deng S S, et al. Preparation of carboxymethylchitosan nanoparticles with acid-sensitive bond based on solid dispersion of 10-hydroxycamptothecin[J]. ISRN Pharmaceutics, 2011, 2011: 624704.
6	梁冉, 冯玉玲, 孙京国.布南色林微米化药物的制备[C]// 中国化学会全国第十一届有机合成化学学术研讨会. 2014.
	Liang R, Feng Y L, Sun J G. Preparation of micronized drug of blonanserin[C]// The 11th National Synthetic Organic Chemistry Symposium. 2014.
7	张海丰, 张鹏宇, 赵贵龙, 等. 纳米二氧化钛的制备及其应用研究进展[J]. 东北电力大学学报, 2014, 34(2): 52-56.
	Zhang H F, Zhang P Y, Zhao G L, et al. Advances on preparation, modification and application of nanosized titanium dioxide[J]. Journal of Northeast Dianli University, 2014, 34(2): 52-56.
8	季璨, 王乃华, 崔峥, 等. 过热液滴闪蒸过程数学模型的建立与应用[J]. 工程热物理学报, 2017, 38(4): 869-875.
	Ji C, Wang N H, Cui Z, et al. The development and application of a mathematical model for superheated droplet flash evaporation[J]. Journal of Engineering Thermophysics, 2017, 38(4): 869-875.
9	Chen Q, Thu K, Bui T D, et al. Development of a model for spray evaporation based on droplet analysis[J]. Desalination, 2016, 399: 69-77.
10	程文龙, 胡磊, 陈华, 等. 真空闪蒸喷雾冷却中非等温液滴闪蒸特性的研究[J]. 真空科学与技术学报, 2015, 35(4): 399-404.
	Cheng W L, Hu L, Chen H, et al. Influence of characteristics of non-isothermal flashing droplet on vacuum flash-spray cooling[J]. Chinese Journal of Vacuum Science and Technology, 2015, 35(4): 399-404.
11	Chen Q, Li Y, Chua K J. On the thermodynamic analysis of a novel low-grade heat driven desalination system[J]. Energy Conversion and Management, 2016, 128: 145-159.
12	Liu X D, Yu L, Zhao L, et al. A comprehensive simulation analysis to optimize the performance of spray evaporator on treating concentrated brine[J]. Desalination, 2023, 548: 116292.
13	Gao H, Wang Q H, Ke X, et al. Preparation and characterization of an ultrafine HMX/NQ co-crystal by vacuum freeze drying method[J]. RSC Advances, 2017, 7(73): 46229-46235.
14	He B B, Tian S H, Ju S H, et al. Preparation of polyphosphoric acid and recovery of valuable fluorine resources through a microwave intensification flash evaporation process[J]. Chemical Engineering and Processing-Process Intensification, 2023, 189: 109397.
15	Risse B, Spitzer D, Hassler D, et al. Continuous formation of submicron energetic particles by the flash-evaporation technique[J]. Chemical Engineering Journal, 2012, 203: 158-165.
16	Pichot V, Seve A, Berthe J E, et al. Study of the elaboration of HMX and HMX composites by the spray flash evaporation process[J]. Propellants, Explosives, Pyrotechnics, 2017, 42(12): 1418-1423.
17	Ghosh M, Sikder A K, Banerjee S, et al. Preparation of reduced sensitivity co-crystals of cyclic nitramines using spray flash evaporation[J]. Defence Technology, 2020, 16(1): 188-200.
18	Ikegami Y, Sasaki H, Gouda T, et al. Experimental study on a spray flash desalination (influence of the direction of injection)[J]. Desalination, 2006, 194(1/2/3): 81-89.
19	刘兵, 宇文璋杰, 杨涛, 等. 异戊烷闪蒸喷雾喷嘴近场雾化与喷嘴内流动特性[J]. 东北电力大学学报, 2022, 42(3): 57-63.
	Liu B, Yuwen Z J, Yang T, et al. Atomization near nozzle filed and internal flow within the nozzle of iso-pentane flashing spray[J]. Journal of Northeast Electric Power University, 2022, 42(3): 57-63.
20	季璨, 王乃华, 崔峥, 等. 高温高压喷雾闪蒸的蒸发特性[J]. 化工学报, 2016, 67(5): 1771-1777.
	Ji C, Wang N H, Cui Z, et al. Evaporation characteristics of spray flash evaporation at high temperature and high pressure[J]. CIESC Journal, 2016, 67(5): 1771-1777.
21	周士鹤, 刘新宇, 冯寅, 等. 基于液滴分析的喷雾闪蒸海水淡化模拟研究[J]. 大连理工大学学报, 2021, 61(6): 593-600.
	Zhou S H, Liu X Y, Feng Y, et al. Simulation study of spray flash evaporation seawater desalination based on droplet analysis[J]. Journal of Dalian University of Technology, 2021, 61(6): 593-600.
22	Cai B A, Zhang Q, Jiang Y, et al. Experimental study on spray flash evaporation under high temperature and pressure[J]. International Journal of Heat and Mass Transfer, 2017, 113: 1106-1115.
23	Loureiro D D, Kronenburg A, Reutzsch J, et al. Droplet size distributions in cryogenic flash atomization[J]. International Journal of Multiphase Flow, 2021, 142: 103705.
24	Mutair S, Ikegami Y. Experimental study on flash evaporation from superheated water jets: influencing factors and formulation of correlation[J]. International Journal of Heat and Mass Transfer, 2009, 52(23/24): 5643-5651.
25	Mutair S, Ikegami Y. On the evaporation of superheated water drops formed by flashing of liquid jets[J]. International Journal of Thermal Sciences, 2012, 57: 37-44.
26	Wang Y, He Q, Yang Q Z, et al. Energy and exergy analyses of circulatory flash evaporation of aqueous NaCl solution[J]. Desalination, 2018, 436: 81-90.
27	Moffat R J. Describing the uncertainties in experimental results[J]. Experimental Thermal and Fluid Science, 1988, 1(1): 3-17.
28	Zeng Y B, Lee C F F. An atomization model for flash boiling sprays[J]. Combustion Science and Technology, 2001, 169(1): 45-67.
29	Oza R D, Sinnamon J F. An experimental and analytical study of flash-boiling fuel injection[C]//SAE Technical Paper Series. Warrendale, PA, United States: SAE International, 1983: 948-962.
30	Sher E, Bar-Kohany T, Rashkovan A. Flash-boiling atomization[J]. Progress in Energy and Combustion Science, 2008, 34(4): 417-439.
31	Bar-Kohany T, Levy M. State of the art review of flash-boiling atomization[J]. Atomization and Sprays, 2016, 26(12): 1259-1305.

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