微通道内液液非均相传质的模拟和实验研究方法进展

doi:10.11949/0438-1157.20240746

摘要/Abstract

摘要：

微通道内液液非均相体系传质行为的研究对明确传质机理，进一步提高传质效率，促进微通道装置在连续流动化学合成、生物医学和溶剂萃取等领域的工业化应用十分重要。介绍了用于微通道内传质研究的指标参数及其影响因素，总结归纳了微通道内液液体系传质研究的技术方法及其相关原理，包括探究两相流动行为、相内传质和相间传质的模拟方法，评价微通道装置整体传质性能的离线实验方法与实时检测微通道内流体速度场和浓度场的在线实验方法，并对未来用于微通道内液液体系传质研究的模拟和实验方法的发展方向提出建议。

关键词: 微通道, 多相流, 传递, 模拟原理, 实验方法

Abstract:

The research of non-equalized system transmission in the microchannel of liquid fluids clarify the mechanism of mass transfer, further improve the efficiency of the quality transmission, and promote the industrialization application of micro-channel devices in the fields of continuous mobile chemical synthesis, biomedical and solvent extraction. The parameters and influencing factors of mass transfer in microchannels are introduced, and the methods and relevant principles are summarized, including the simulation methods for exploring two-phase flow behavior, in-phase and interphase mass transfer, the offline experimental method for evaluating the overall mass transfer performance of microchannel devices, and the online experimental method for real-time detection of the fluid velocity and concentration field in microchannels. The possible development of simulation and experimental methods for the study of mass transfer in liquid-liquid systems in microchannels is also proposed.

Key words: microchannel, multiphase flow, transport, simulation principle, experimental method

中图分类号:

TQ 027.3

张鑫源, 何呈祥, 李亚婷, 朱春英, 马友光, 付涛涛. 微通道内液液非均相传质的模拟和实验研究方法进展[J]. 化工学报, 2025, 76(2): 484-503.

Xinyuan ZHANG, Chengxiang HE, Yating LI, Chunying ZHU, Youguang MA, Taotao FU. Advances in simulation and experimental research methods for mass transfer of liquid-liquid heterogeneous system in microchannels[J]. CIESC Journal, 2025, 76(2): 484-503.

图/表 18

图1 不同流型的图像

Fig.1 Images of different flow patterns

图2 液滴形状近似图[19]

Fig.2 Approximate diagram of droplet shape[19]

表1 常用的无量纲数

Table1 Commonly used dimensionless numbers

无量纲数	定义式	物理意义
毛细数（Ca）	$C a = \frac{μ u}{σ}$	表征黏性力与界面张力的相对大小
Reynolds数（Re）	$R e = \frac{ρ u d_{h}}{μ}$	表征惯性力与黏性力的相对大小
Weber数（We）	$W e = \frac{ρ u^{2} d_{h}}{σ}$	表征惯性力与界面张力的相对大小

表1 常用的无量纲数

Table1 Commonly used dimensionless numbers

无量纲数	定义式	物理意义
毛细数（Ca）	$C a = \frac{μ u}{σ}$	表征黏性力与界面张力的相对大小
Reynolds数（Re）	$R e = \frac{ρ u d_{h}}{μ}$	表征惯性力与黏性力的相对大小
Weber数（We）	$W e = \frac{ρ u^{2} d_{h}}{σ}$	表征惯性力与界面张力的相对大小

表2 液膜厚度预测式

Table 2 Liquid film thickness prediction formula

预测式

变量意义

文献

h = 1.34 R C a^{2 / 3} = 1.34 R \frac{μ_{C H} V_{s}}{σ_{C H}}

μ_CH——环己烷黏度，Pa·s

V_s——段塞速度，m/s

σ_CH——环己烷-水的界面张力，N/m

[21]

$\frac{δ}{d} = 0.329 C a_{m i x}^{0.6409} R e_{m i x}^{0.1067}$

$C a_{m i x} = \frac{μ_{c} u_{m i x}}{γ}$

$R e_{m i x} = \frac{ρ_{c} d u_{m i x}}{μ_{c}}$

δ——膜厚，mm

d——微通道直径，mm

μ_c——连续相黏度，Pa·s

ρ_c——连续相密度，kg/m³

u_mix——两相总流速，m/s

γ——界面张力，N/m

[22]

$\frac{h}{R} = 0.35 C a^{0.354} W e^{0.097}$

$C a = \frac{μ u}{σ}$

$W e = \frac{ρ u^{2} d_{h}}{σ}$

ρ——连续相密度，kg/m³

μ——连续相黏度，Pa·s

d_h——微通道直径，mm

[23]

表2 液膜厚度预测式

Table 2 Liquid film thickness prediction formula

预测式

变量意义

文献

h = 1.34 R C a^{2 / 3} = 1.34 R \frac{μ_{C H} V_{s}}{σ_{C H}}

μ_CH——环己烷黏度，Pa·s

V_s——段塞速度，m/s

σ_CH——环己烷-水的界面张力，N/m

[21]

$\frac{δ}{d} = 0.329 C a_{m i x}^{0.6409} R e_{m i x}^{0.1067}$

$C a_{m i x} = \frac{μ_{c} u_{m i x}}{γ}$

$R e_{m i x} = \frac{ρ_{c} d u_{m i x}}{μ_{c}}$

δ——膜厚，mm

d——微通道直径，mm

μ_c——连续相黏度，Pa·s

ρ_c——连续相密度，kg/m³

u_mix——两相总流速，m/s

γ——界面张力，N/m

[22]

$\frac{h}{R} = 0.35 C a^{0.354} W e^{0.097}$

$C a = \frac{μ u}{σ}$

$W e = \frac{ρ u^{2} d_{h}}{σ}$

ρ——连续相密度，kg/m³

μ——连续相黏度，Pa·s

d_h——微通道直径，mm

[23]

图3 液滴/段塞内循环

Fig.3 Internal circulation of droplets or slug plugs

图4 基于双膜理论的非均相传质机理示意图

Fig.4 Schematic diagram of mass transfer mechanism for heterogeneous system based on double film theory

表3 微通道内平均体积传质系数预测式

Table 3 Prediction formula of average volume mass transfer coefficient in microchannel

预测式	微通道装置	文献
$K_{L} a τ = C a^{- 0.09} R e^{- 0.09} {(\frac{D}{L})}^{- 0.1}$	直微通道	[26]
$K_{L} a τ = 0.88 C a^{- 0.09} R e^{- 0.09} {(\frac{D}{L})}^{- 0.1}$	并行直微通道	[26]
$K_{L} a = {(0.84998 + 0.35556 q^{- 1} + 25.795 U_{t}^{- 1})}^{- 1}$	蛇形微通道（D_h=319 μm）	[27]
$K_{L} a = - 1.2092 \times 10^{- 4} q^{- 1} + 0.051939 U_{t} - 0.075017 U_{t}^{4}$	分裂重组微通道（D_h=184 μm）	[27]
$K_{L} a = 0.03 {(1 + \frac{1}{q})}^{2.3} R e^{1.4}$	T型微通道	[28]
$K_{L} a = 0.06 {(1 + \frac{1}{q})}^{2.3} R e^{1.1}$	十字聚焦微通道	[28]

表3 微通道内平均体积传质系数预测式

Table 3 Prediction formula of average volume mass transfer coefficient in microchannel

预测式	微通道装置	文献
$K_{L} a τ = C a^{- 0.09} R e^{- 0.09} {(\frac{D}{L})}^{- 0.1}$	直微通道	[26]
$K_{L} a τ = 0.88 C a^{- 0.09} R e^{- 0.09} {(\frac{D}{L})}^{- 0.1}$	并行直微通道	[26]
$K_{L} a = {(0.84998 + 0.35556 q^{- 1} + 25.795 U_{t}^{- 1})}^{- 1}$	蛇形微通道（D_h=319 μm）	[27]
$K_{L} a = - 1.2092 \times 10^{- 4} q^{- 1} + 0.051939 U_{t} - 0.075017 U_{t}^{4}$	分裂重组微通道（D_h=184 μm）	[27]
$K_{L} a = 0.03 {(1 + \frac{1}{q})}^{2.3} R e^{1.4}$	T型微通道	[28]
$K_{L} a = 0.06 {(1 + \frac{1}{q})}^{2.3} R e^{1.1}$	十字聚焦微通道	[28]

图5 不同形式的微通道结构

Fig.5 Different forms of microchannel structures

图6 不同障碍形状微通道内的体积分数云图和速度矢量图[52]

Fig.6 Volume fraction cloud and velocity vector image in microchannels with different obstacle shapes[52]

图7 两种混合模式[54]

Fig.7 Two modes of mixing[54]

图8 三维计算域中X-Y平面上液滴内外的网格划分情况和流体的流线图[55]

Fig.8 Mesh division inside and outside droplet and streamline in X-Y plane of computational domain[55]

表4 微通道内液液非均相体系传质研究所用的模拟方法、通道装置和主要研究内容

Table 4 Simulation methods， channel devices and main research contents for mass transfer of liquid-liquid heterogeneous systems in microchannels

类型	微通道装置	模拟方法	研究内容	文献
两相流	具有突然扩张/收缩腔的微通道	VOF	微腔通道内液液两相流速、液滴形状和流场涡度的演变情况	[60]
两相流	周期膨胀微通道	LSM	微腔通道内流动液滴的内循环情况	[61]
相内传质	十字聚焦微通道	VOF+UDS	微通道内表观流速对混合效率的影响	[62]
	T型微通道	VOF+SMT	黏度比对微通道内液滴内循环的影响	[63]
	蛇形微通道	VOF+UDS	弯曲半径和分散相分数对液滴内混合的影响	[64]
	带有内壁脊的蛇形微通道	VOF+SMT	微通道内液滴内混合的机理以及脊宽和脊数对不同尺寸液滴内部混合的影响	[65]
	凹凸蛇形微通道	VOF+SMT	凹凸结构尺寸、布局和数量对液滴内部混合的影响	[66]
	T结正弦微通道	VOF+SMT	促进液滴内部混合的机理和混合效率探究	[67]
	蛇形微通道	VOF+MTE	不同通道截面形状和通道截面横向比对液滴内部混合效率和反应效果的影响	[68]
相间传质	T型微通道	VOF+C-CST	不同流型下进行萃取的传质机理和效果研究	[69]
	十字聚焦微通道	VOF+UDF	微通道内部分互溶体系的液滴形成机理、传质机理以及弯曲通道增强传质机理的研究	[70]
	固定液滴形状的微通道计算域	MTE	通道尺寸和操作条件对界面面积、萃取效率、体积传质系数和双相反应的影响	[71]
	含SK内构件的T型微通道	EMP+PBE+SMT	不同流速下微通道内液滴的动态尺寸分布、流体动力学行为和传质行为研究	[72]

表5 各种实验方法的特点、适用范围、测量尺度和响应时间

Table 5 Characteristics， applicability， measurement scales， and response times of various experimental methods

实验方法	特点及适用范围	测量尺度	响应时间	文献
反应法	离线检测方法，过程简单，操作容易，适用性强，可测定微通道装置整体的传质系数；通常选择中和、皂化或碱性水解等快速反应消除化学反应对传质过程的强化作用，可用于微通道装置整体传质性能的评价	毫米/厘米级	秒级	[19,73-74]
萃取法	离线检测方法，特点与反应法相似，但是为物理过程，通过物质在两相间的传递测定微通道装置整体的传质系数；由于通道出口处两相不能及时分离，需采用外推法排除此过程两相间传质的影响，获得出口处目标相内传递物质的平均浓度	毫米/厘米级	秒级	[75-77]
微分辨荧光诱导技术	测量快，波动小，灵敏度高，可获得单一平面液层内的浓度信息；但是设备昂贵，普适性弱，针对不同物系和微通道装置需重新标定荧光强度与物质浓度的关系，并且存在相间荧光强度的交叉干扰；常用于微通道内段塞流型下浓度场的实时监测	微米/毫米级	微秒/毫秒级	[28,78-80]
比色技术	检测迅速，响应及时，较微分辨荧光诱导技术更实用，且更易实施；需根据特定的研究体系构建灰度与物质浓度的标准曲线，获取的浓度信息为多平面液层叠加后的结果；适于微通道内对称流动下浓度场的实时监测	微米/毫米级	微秒/毫秒级	[81-83]
微粒成像测速技术	所用设备与微分辨荧光诱导技术类似，需根据测量尺度和操作条件选择合适的示踪剂粒径、浓度和激光脉冲时间间隔；示踪剂微粒的布朗运动会对速度求算产生影响，通过对多个示踪微粒速度的总体平均可减弱误差；该技术不适合数微米或纳米尺度下流体速度场的实时监测，因为此时与测量尺度适配的示踪微粒的剧烈布朗运动会导致流体速度求算的显著偏差	微米/毫米级	微秒/毫秒级	[84-86]

表5 各种实验方法的特点、适用范围、测量尺度和响应时间

Table 5 Characteristics， applicability， measurement scales， and response times of various experimental methods

实验方法	特点及适用范围	测量尺度	响应时间	文献
反应法	离线检测方法，过程简单，操作容易，适用性强，可测定微通道装置整体的传质系数；通常选择中和、皂化或碱性水解等快速反应消除化学反应对传质过程的强化作用，可用于微通道装置整体传质性能的评价	毫米/厘米级	秒级	[19,73-74]
萃取法	离线检测方法，特点与反应法相似，但是为物理过程，通过物质在两相间的传递测定微通道装置整体的传质系数；由于通道出口处两相不能及时分离，需采用外推法排除此过程两相间传质的影响，获得出口处目标相内传递物质的平均浓度	毫米/厘米级	秒级	[75-77]
微分辨荧光诱导技术	测量快，波动小，灵敏度高，可获得单一平面液层内的浓度信息；但是设备昂贵，普适性弱，针对不同物系和微通道装置需重新标定荧光强度与物质浓度的关系，并且存在相间荧光强度的交叉干扰；常用于微通道内段塞流型下浓度场的实时监测	微米/毫米级	微秒/毫秒级	[28,78-80]
比色技术	检测迅速，响应及时，较微分辨荧光诱导技术更实用，且更易实施；需根据特定的研究体系构建灰度与物质浓度的标准曲线，获取的浓度信息为多平面液层叠加后的结果；适于微通道内对称流动下浓度场的实时监测	微米/毫米级	微秒/毫秒级	[81-83]
微粒成像测速技术	所用设备与微分辨荧光诱导技术类似，需根据测量尺度和操作条件选择合适的示踪剂粒径、浓度和激光脉冲时间间隔；示踪剂微粒的布朗运动会对速度求算产生影响，通过对多个示踪微粒速度的总体平均可减弱误差；该技术不适合数微米或纳米尺度下流体速度场的实时监测，因为此时与测量尺度适配的示踪微粒的剧烈布朗运动会导致流体速度求算的显著偏差	微米/毫米级	微秒/毫秒级	[84-86]

图9 微通道内水相段塞随时间的变化情况[73]

Fig.9 Changes of water phase slug in microchannels over time[73]

图10 传质研究的实验流程和人形微通道单元的具体构型[87]

Fig.10 Scheme of mass transfer research and specific configuration of humanoid microchannel unit[87]

表6 萃取法研究微通道内液液非均相体系传质过程所用的物系、装置和主要研究内容

Table 6 System and device used in extraction method to study mass transfer process of liquid-liquid heterogeneous system in microchannels and main research contents

研究物系	微通道装置	研究内容	文献
甲苯-乙酸-水	导线嵌入式同心微通道	流率、相比、初始乙酸浓度、嵌件形状和流型对传质的影响	[90]
甲苯-乙酸-水	T型直通道 T型螺旋通道	流速、通道直径、通道结构和机械振动对流型和传质的影响	[75]
甲苯+N1932-钒离子-水	Raydrop微通道装置	硫酸浓度和铬离子对界面和不同钒离子物种传质的影响	[91]
正丁醇-琥珀酸-水	垂直T型微通道逆流萃取装置	相比、总流速和主通道内径对平均液滴直径、萃取效率和体积传质系数的影响	[92]
正辛醇-丙酸-水	具有入口凹坑结构和主通道凹坑阵列的T型微通道	T型结处的凹坑直径、混合通道内的凹坑设计以及通道直径对传质系数和萃取效率的影响	[93]
正辛醇-茜红素S-水	多环微通道	环直径、环数和环间距对传质的影响以及基于人工智能模型对萃取性能的准确预测	[94]
正辛烷+正辛醇-苯酚-水	非对称阶跃T结微通道	对比了阶跃T结微通道与常规T型微通道的传质性能，提出一种采样检测方法量化液滴形成阶段和运动阶段的贡献	[95]
十二烷-苯酚-水	T型微通道	不同流型下的传质研究和机理分析	[76]
十二烷-苯酚-水	T型微通道	液滴长度、截面形状和当量通道直径对体积传质系数的影响	[37]
正己烷-丙酸-水	T型并行微通道	研究了并行微通道内的段塞形成、段塞体积、比表面积、萃取效率和传质系数，并与单通道进行了对比	[96]
磷酸二（2-乙基己）酯+煤油-Cu²⁺-水	具有变形插入物的微通道	总流速、微通道内径、插入物直径和萃取液浓度对萃取效率和传质系数的影响	[97]
乙酸乙酯-水	T型微通道	微通道直径、水相流速和温度对乙酸乙酯在水相中传质系数的影响	[77]
TBP+煤油-磷酸-水	旋转螺旋微通道	流率、转速、平均液滴直径和平均停留时间对旋转螺旋微通道传质性能的影响与传质系数预测式的建立	[98]

表6 萃取法研究微通道内液液非均相体系传质过程所用的物系、装置和主要研究内容

Table 6 System and device used in extraction method to study mass transfer process of liquid-liquid heterogeneous system in microchannels and main research contents

研究物系	微通道装置	研究内容	文献
甲苯-乙酸-水	导线嵌入式同心微通道	流率、相比、初始乙酸浓度、嵌件形状和流型对传质的影响	[90]
甲苯-乙酸-水	T型直通道 T型螺旋通道	流速、通道直径、通道结构和机械振动对流型和传质的影响	[75]
甲苯+N1932-钒离子-水	Raydrop微通道装置	硫酸浓度和铬离子对界面和不同钒离子物种传质的影响	[91]
正丁醇-琥珀酸-水	垂直T型微通道逆流萃取装置	相比、总流速和主通道内径对平均液滴直径、萃取效率和体积传质系数的影响	[92]
正辛醇-丙酸-水	具有入口凹坑结构和主通道凹坑阵列的T型微通道	T型结处的凹坑直径、混合通道内的凹坑设计以及通道直径对传质系数和萃取效率的影响	[93]
正辛醇-茜红素S-水	多环微通道	环直径、环数和环间距对传质的影响以及基于人工智能模型对萃取性能的准确预测	[94]
正辛烷+正辛醇-苯酚-水	非对称阶跃T结微通道	对比了阶跃T结微通道与常规T型微通道的传质性能，提出一种采样检测方法量化液滴形成阶段和运动阶段的贡献	[95]
十二烷-苯酚-水	T型微通道	不同流型下的传质研究和机理分析	[76]
十二烷-苯酚-水	T型微通道	液滴长度、截面形状和当量通道直径对体积传质系数的影响	[37]
正己烷-丙酸-水	T型并行微通道	研究了并行微通道内的段塞形成、段塞体积、比表面积、萃取效率和传质系数，并与单通道进行了对比	[96]
磷酸二（2-乙基己）酯+煤油-Cu²⁺-水	具有变形插入物的微通道	总流速、微通道内径、插入物直径和萃取液浓度对萃取效率和传质系数的影响	[97]
乙酸乙酯-水	T型微通道	微通道直径、水相流速和温度对乙酸乙酯在水相中传质系数的影响	[77]
TBP+煤油-磷酸-水	旋转螺旋微通道	流率、转速、平均液滴直径和平均停留时间对旋转螺旋微通道传质性能的影响与传质系数预测式的建立	[98]

图11 运用micro-LIF技术研究微通道内非均相液液体系传质过程的典型实验装置示意图[28]

Fig.11 Schematic diagram of typical experimental device for studying mass transfer process of heterogeneous liquid systems in microchannels using micro-LIF technology [28]

图12 micro-PIV实验装置图和可视化实验结果[102]

Fig.12 Experimental setup diagram and visualized experimental results of micro-PIV[102]

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