WO2021087953A1 - 液滴镊子以及液滴控制方法 - Google Patents

液滴镊子以及液滴控制方法 Download PDF

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WO2021087953A1
WO2021087953A1 PCT/CN2019/116589 CN2019116589W WO2021087953A1 WO 2021087953 A1 WO2021087953 A1 WO 2021087953A1 CN 2019116589 W CN2019116589 W CN 2019116589W WO 2021087953 A1 WO2021087953 A1 WO 2021087953A1
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droplet
tweezers
hydrophobic
angle
liquid droplet
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PCT/CN2019/116589
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English (en)
French (fr)
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黄海波
卞雄恒
陈立国
孙立宁
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苏州大学
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01L—CHEMICAL OR PHYSICAL LABORATORY APPARATUS FOR GENERAL USE
    • B01L3/00—Containers or dishes for laboratory use, e.g. laboratory glassware; Droppers
    • B01L3/50—Containers for the purpose of retaining a material to be analysed, e.g. test tubes
    • B01L3/502—Containers for the purpose of retaining a material to be analysed, e.g. test tubes with fluid transport, e.g. in multi-compartment structures
    • B01L3/5027—Containers for the purpose of retaining a material to be analysed, e.g. test tubes with fluid transport, e.g. in multi-compartment structures by integrated microfluidic structures, i.e. dimensions of channels and chambers are such that surface tension forces are important, e.g. lab-on-a-chip
    • B01L3/502769—Containers for the purpose of retaining a material to be analysed, e.g. test tubes with fluid transport, e.g. in multi-compartment structures by integrated microfluidic structures, i.e. dimensions of channels and chambers are such that surface tension forces are important, e.g. lab-on-a-chip characterised by multiphase flow arrangements
    • B01L3/502784—Containers for the purpose of retaining a material to be analysed, e.g. test tubes with fluid transport, e.g. in multi-compartment structures by integrated microfluidic structures, i.e. dimensions of channels and chambers are such that surface tension forces are important, e.g. lab-on-a-chip characterised by multiphase flow arrangements specially adapted for droplet or plug flow, e.g. digital microfluidics
    • B01L3/502792—Containers for the purpose of retaining a material to be analysed, e.g. test tubes with fluid transport, e.g. in multi-compartment structures by integrated microfluidic structures, i.e. dimensions of channels and chambers are such that surface tension forces are important, e.g. lab-on-a-chip characterised by multiphase flow arrangements specially adapted for droplet or plug flow, e.g. digital microfluidics for moving individual droplets on a plate, e.g. by locally altering surface tension
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01L—CHEMICAL OR PHYSICAL LABORATORY APPARATUS FOR GENERAL USE
    • B01L3/00—Containers or dishes for laboratory use, e.g. laboratory glassware; Droppers
    • B01L3/56—Labware specially adapted for transferring fluids
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01L—CHEMICAL OR PHYSICAL LABORATORY APPARATUS FOR GENERAL USE
    • B01L2200/00—Solutions for specific problems relating to chemical or physical laboratory apparatus
    • B01L2200/06—Fluid handling related problems
    • B01L2200/0621—Control of the sequence of chambers filled or emptied
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01L—CHEMICAL OR PHYSICAL LABORATORY APPARATUS FOR GENERAL USE
    • B01L2300/00—Additional constructional details
    • B01L2300/16—Surface properties and coatings
    • B01L2300/161—Control and use of surface tension forces, e.g. hydrophobic, hydrophilic
    • B01L2300/165—Specific details about hydrophobic, oleophobic surfaces

Definitions

  • the invention belongs to the technical field of micro-droplet control, and relates to a droplet tweezers and a droplet control method.
  • the surface microfluidic technology based on droplets due to its open structural characteristics, is beneficial to compatibility with other detection and experimental methods, and has been widely used in microfluidic systems, droplet transfer, microreactors, and biomedical fields. .
  • CAH contact angle hysteresis
  • surface contamination and liquid loss will be inevitable.
  • non-destructive droplet manipulation methods on superhydrophobic surfaces have attracted widespread attention.
  • the existing non-destructive droplet transfer methods are mainly based on smart surfaces with adjustable adhesion. By switching the high adhesion force to capture the droplets and switching the low adhesion force to release the droplets, the transfer of the droplets is realized.
  • the most commonly used method is to treat the surface with special materials so that the surface can respond to external stimuli and change its surface adhesion characteristics.
  • external stimuli will reduce the biological activity of the droplets and increase the complexity of the operation.
  • some people have also proposed a method of transporting droplets by looking for flexible surface materials that can be stretched or bent.
  • a droplet tweezers including:
  • Two hydrophobic plates are respectively fixed to the head ends of the two tweezers arms; the two hydrophobic plates are arranged at an angle; the two hydrophobic plates can move relatively in translation, and the angle between the two hydrophobic plates Adjustable.
  • the above-mentioned droplet tweezers can change the direction and size of the capillary force on the droplet through the change of the hydrophobic non-parallel plate structure, which can realize the upward movement of the droplet and the downward movement of the droplet, thereby realizing the capture of the droplet/ freed.
  • Different from other droplet capture/release methods since the force of this type of capture/release droplet comes from the structural characteristics of the non-parallel plate itself, it shows wide applicability and superiority for the hydrophobic nature of different bottom surfaces.
  • the compatibility of biology and chemistry can become a powerful platform for microfluidic systems, droplet transportation, biological analysis, and microreaction vessels.
  • the hydrophobic plate includes a glass substrate and a hydrophobic layer covering the glass substrate.
  • the hydrophobic layer is a Teflon layer.
  • the contact angle of the hydrophobic layer is 120 degrees, and the CAH is 10 degrees.
  • the thickness of the hydrophobic layer is 100 ⁇ m.
  • the thickness of the glass substrate is 150 ⁇ m; the length and width of the glass substrate are both 5 cm.
  • the second object of the present invention is to provide a droplet control method.
  • a droplet control method adopts the droplet tweezers provided by the present invention
  • the above-mentioned droplet control method adopts the droplet tweezers provided by the present invention.
  • the direction and size of the capillary force on the droplet can be changed through the change of the hydrophobic non-parallel plate structure, which can realize the upward direction of the droplet and the direction of the droplet. Move down to achieve the capture/release of droplets.
  • Different from other droplet capture/release methods since the force of this type of capture/release droplet comes from the structural characteristics of the non-parallel plate itself, it shows wide applicability and superiority for the hydrophobic nature of different bottom surfaces.
  • the compatibility of biology and chemistry can become a powerful platform for microfluidic systems, droplet transportation, biological analysis, and microreaction vessels.
  • the tip gap L n of the tweezers arm of the droplet tweezers satisfies the following conditions:
  • ⁇ a is the advancing angle of the interface of the droplet tweezers
  • ⁇ is the angle between the hydrophobic plate of the droplet tweezers and the vertical direction
  • R is the spherical radius of the droplet.
  • H is the minimum height of the droplet tweezers from the bottom surface
  • L w forceps liquid droplet width end of the bridge ⁇ a is the advancing angle of the liquid droplet interface tweezers
  • ⁇ a surface contact angle of the hydrophobic droplet forceps plate ⁇ is the angle between the hydrophobic plate of the droplet tweezers and the vertical direction.
  • the included angle of the droplet tweezers is increased so that the included angle is greater than 29 degrees.
  • FIG. 1 is a schematic diagram of the structure of a droplet tweezers according to an embodiment of the present invention.
  • FIG. 2 is a schematic diagram of the structure of the hydrophobic plate of the droplet tweezers in FIG. 1.
  • Figure 3 is a schematic diagram of the droplet capture process.
  • Figure 4 is a schematic diagram of the droplet release process.
  • Figure 5 shows the force and movement trend analysis diagram of the droplet in the non-parallel plate under the condition of the non-parallel plate being squeezed/stretched and the experimental result diagram.
  • Fig. 6 is a graph showing the force and movement trend analysis of droplets in the non-parallel plate when the non-parallel plate is closed/opened and the experimental results.
  • Figure 7 shows the droplets in different The movement trend graph at the time of and ⁇ .
  • Figure 8 shows the droplets in different The movement trend graph at the time of and ⁇ .
  • Figure 9 shows the droplets in different The movement trend graph at the time of and ⁇ .
  • the inventor of the present invention found that the change of the hydrophobic non-parallel plate structure can not only change the size of the Lagrangian force on the droplet, but also change the direction of the Lagrangian force on the droplet.
  • the droplet movement is mainly affected by two forces.
  • the first is the asymmetric Lagrangian force caused by the structure, which causes the droplet to move and determines the direction of the droplet's movement.
  • the second is the hysteresis force caused by contact angle hysteresis (CAH), which hinders the movement of the droplet and determines whether the droplet can move under the action of Lagrangian force.
  • CAH contact angle hysteresis
  • the Lagrangian force generated by the structure is determined by two factors.
  • the first is the width L n at the bottom of the liquid bridge in the non-parallel structure.
  • L n the width of the liquid bridge in the non-parallel structure.
  • the second is the angle ⁇ between the hydrophobic plate and the vertical. The influence of these two factors on the direction of droplet movement is analyzed through geometric structure and Laplace equation.
  • the hydrophobic non-parallel plate model is shown in Figure 5.
  • the contact angle (CA) at the bottom of the liquid bridge is ⁇ 1
  • the contact angle at the upper end is ⁇ 2
  • the length of the liquid bridge is D
  • the distance between the intersection point between the bottom of the liquid bridge and the non-parallel plate is S
  • the liquid in the bridge The volume of the drop can be expressed as:
  • the present invention provides a droplet tweezers, which includes two tweezers arms 10 and two hydrophobic plates 20.
  • the main function of the tweezers arm 10 is to support the hydrophobic plate 20 and drive the hydrophobic plate 20 to move, thereby realizing the mutual translational opening and closing action of the two hydrophobic plates 20 and rotating around the intersection of the extension lines of the two hydrophobic plates 20 The opening and closing action.
  • the main function of the hydrophobic plate 20 is to rely on the mutual translational opening and closing action of the two hydrophobic plates 20 and the opening and closing action of rotating around the intersection of the extension lines of the two hydrophobic plates 20, so as to achieve different effects on the droplets. Power, and then achieve the capture or release of droplets. When the droplet tweezers capture or release the droplet, the tweezers arm 10 does not contact the droplet, and the hydrophobic plate 20 directly contacts the droplet.
  • the surfaces of the two hydrophobic plates are hydrophobic in nature.
  • Two hydrophobic plates are respectively fixed to the head ends of the two forceps arms; that is, one hydrophobic plate is located at the head end of one forceps arm, and the other hydrophobic plate is located at the head end of the other forceps arm.
  • the two hydrophobic plates are arranged at an angle, that is, the two hydrophobic plates are not parallel, that is, the two hydrophobic plates form a non-parallel plate structure.
  • the two drain plates can move relatively in parallel, that is, the two drain plates can realize the opening and closing action of mutual translation; and the angle between the two drain plates can be adjusted, that is, the two drain plates can be realized around the two drain plates.
  • the opening and closing action of the rotation of the intersection of the extension lines of the two hydrophobic plates are hydrophobic in nature.
  • the specific structure of the hydrophobic plate is as follows: the hydrophobic plate includes a glass substrate and a hydrophobic layer covered on the glass substrate.
  • the function of the hydrophobic layer is mainly to make the hydrophobic plate exhibit hydrophobic properties, and the glass substrate is used as the substrate.
  • the thickness of the glass substrate is 150 ⁇ m.
  • the length and width of the glass substrate are both 5 cm.
  • the hydrophobic layer is a Teflon layer.
  • the Teflon layer has good hydrophobic properties, which can further expand the use of droplet tweezers.
  • the above-mentioned hydrophobic plate can be prepared in the following manner: dipping a glass sheet in a Teflon melt, and then heating the solid film layer at 160 degrees on a hot plate for 30 minutes.
  • the contact angle of the hydrophobic layer is 120 degrees, and the CAH is 10 degrees. This can have good hydrophobic properties, and can further expand the use of droplet tweezers.
  • the thickness of the hydrophobic layer is preferably 100 ⁇ m.
  • the present invention is not limited to the glass substrate, and other materials can also be used as the substrate.
  • the hydrophobic layer is not limited to the Teflon layer, and may also be a hydrophobic layer made of other materials.
  • the hydrophobic plate can also be integrated, that is, the hydrophobic plate is directly made of a hydrophobic material, or the surface microstructure of the substrate directly makes the surface hydrophobic.
  • the invention also provides a droplet control method.
  • a droplet control method adopts the droplet tweezers provided by the present invention
  • the droplet tweezers approach the droplet vertically downwards, and then part of the droplet enters the tweezers to form a liquid bridge (Figure 3a-b).
  • the droplet can be completely entered into the droplet tweezers (de in Figure 3).
  • R is the spherical radius of the drop on the open surface
  • L Ini is the width of the tip of the initial droplet tweezers.
  • the second step is inevitable, so there is no requirement for control parameters. This conclusion is explained from a theoretical perspective.
  • the part inside the liquid tweezers is defined as Part 1, where the pressure is P 1 ; the part under the liquid tweezers is Part 2, where the pressure is P 2 . Therefore, P 1 and P 2 can be calculated using the following equation:
  • L w tweezers liquid droplet bridge end width, H is the height from the bottom surface of the droplet tweezers.
  • H is mainly restricted by the third step. If it is necessary to separate the droplet from the bottom surface, the adhesion force should be overcome. In order to reduce this adhesion force, the droplet is squeezed to reduce the contact area, that is, to reduce the length of the contact line on the bottom surface. In order to accomplish this step, leakage should be avoided.
  • the value of L Final needs to be small. If the droplet of Part 1 can overcome the resistance of CAH and move upward after being squeezed, it will move the droplet away from the bottom plate (at this time, due to the small contact area of the bottom surface, the adhesion is small, V part1 ⁇ V). Therefore, according to the previous analysis, it can be obtained that when the ⁇ is different, the droplet can overcome the CAH and completely enter the droplet tweezers. Range (the part under the solid line in Figure 9). By measuring the different ⁇ conditions, when the droplet completely enters the droplet tweezers To confirm this theoretical result (the Yonzi mark point in Figure 9). It is found that these points are below the solid line, and the experimental results are in good agreement with the theoretical analysis.
  • the release process is analyzed below.
  • a droplet tweezers with a thickness of 100 ⁇ m and a Teflon cover are preferred to ensure that the droplet can fall by gravity when it is greater than 0.8 microliters.
  • the tip gap L n of the tweezers arm of the droplet tweezers satisfies the following conditions:
  • ⁇ a is the advancing angle of the interface of the droplet tweezers
  • ⁇ is the angle between the hydrophobic plate of the droplet tweezers and the vertical direction
  • R is the spherical radius of the droplet.
  • H is the minimum height of the droplet tweezers from the bottom surface
  • L w forceps liquid droplet width end of the bridge ⁇ a is the advancing angle of the liquid droplet interface tweezers
  • ⁇ a surface contact angle of the hydrophobic droplet forceps plate ⁇ is the angle between the hydrophobic plate of the droplet tweezers and the vertical direction.
  • the included angle of the droplet tweezers is increased so that the included angle is greater than 29 degrees.
  • the following describes the method for capturing or releasing droplets by the droplet tweezers of the present invention.
  • Capture process First, select the appropriate initial gap of the droplet tweezers according to the size of the droplet, and place the droplet tweezers vertically downward (Figure 3-a), make the two hydrophobic plates close to the droplet and contact with the droplet, so that the two A liquid bridge is formed in the hydrophobic plate ( Figure 3-b); after that, choose a suitable droplet tweezers to press the height, and continue to move the two hydrophobic plates downward so that the droplets can enter between the two hydrophobic plates more (Figure 3).
  • the above-mentioned droplet tweezers can change the direction and size of the capillary force on the droplet through the change of the hydrophobic non-parallel plate structure, which can realize the upward movement of the droplet and the downward movement of the droplet, thereby realizing the capture of the droplet/ freed.
  • Different from other droplet capture/release methods since the force of this type of capture/release droplet comes from the structural characteristics of the non-parallel plate itself, it shows wide applicability and superiority for the hydrophobic nature of different bottom surfaces.
  • the compatibility of biology and chemistry can become a powerful platform for microfluidic systems, droplet transportation, biological analysis, and microreaction vessels.
  • the invention also provides a droplet capturing and releasing device.
  • a droplet capturing and releasing device includes:
  • the droplet tweezers are the droplet tweezers provided by the present invention.
  • the translation mechanism is connected to the tail end of the forceps arm of the droplet forceps and controls the translational opening and closing of the forceps arm;
  • a rotating mechanism which is connected to the tail end of the forceps arm and controls the rotating opening and closing of the forceps arm.
  • the main function of the translation mechanism is to control the opening and closing movement of the tweezers arms to move in parallel to each other, thereby realizing the opening and closing movement of the hydrophobic plates to move in parallel to each other.
  • the main function of the rotating mechanism is to control the opening and closing movement of the relative rotation of the tweezers arm, thereby realizing the opening and closing movement of the two hydrophobic plates rotating around the intersection of the extension lines of the two hydrophobic plates. .
  • the translation mechanism is a miniature electric clamp.
  • the precision control of the miniature electric clamp can be 0.2 microns, and the control is more precise.
  • the droplet capture and release device also includes an XYZ three-axis control platform, and the miniature electric clamp is installed on the XYZ three-axis control platform.
  • the XYZ three-axis control platform realizes the positioning of the droplet capture and release process; among them, the position of the droplet on the bottom surface is controlled by XY (the accuracy is preferably controlled to 0.2 microns), and the z-axis is used to control the droplet tweezers to capture the droplet.
  • the height of the droplet tweezers (its accuracy is preferably controlled to 0.2 microns).
  • the end of the forceps arm 10 is provided with a rotating waist hole 11. This can help control the opening and closing action of the hydrophobic plate rotating around the intersection of the extension lines of the two hydrophobic plates.
  • the accuracy is preferably controlled to 1°.
  • the above-mentioned droplet capture and release device adopts the droplet tweezers provided by the present invention.
  • the direction and size of the capillary force on the droplet can be changed through the change of the hydrophobic non-parallel plate structure, which can realize the upward movement of the droplet and the realization of the droplet Move downwards to achieve the capture/release of droplets.
  • Different from other droplet capture/release methods since the force of this capture/release droplet comes from the structural characteristics of the non-parallel plate itself, it has shown wide applicability for the hydrophobic nature of different bottom surfaces and can become a micro A powerful platform for fluid systems, droplet transportation, biological analysis, micro-reaction vessels, etc.

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Abstract

一种液滴镊子及液滴控制方法。液滴镊子包括：两个镊臂；两个疏水板，分别固定于两个镊臂的头端；两个疏水板能够相对平动，且两个疏水板之间的角度可调。通过疏水不平行板结构变化，液滴镊子可以改变液滴所受毛细管力的方向和大小，既能实现液滴的向上运动又能实现液滴的向下运动，从而实现了液滴的捕获/释放，由于捕获/释放液滴的力来自于疏水不平行板本身的结构特性，所以液滴镊子具有广泛适用性和生物兼容性，可以应用于微流体系统、液滴输送、生物分析、微反应容器等方面。

Description

液滴镊子以及液滴控制方法 技术领域
本发明属于微液滴控制技术领域，涉及一种液滴镊子以及液滴控制方法。
背景技术
目前，基于液滴的表面微流体技术，由于其开放式的结构特性，有利于兼容其它检测和实验手段，在微流体系统、液滴转移、微反应器、生物医学领域等方面得到了广泛应用。然而，由于接触角滞后(CAH)和接触线固定等原因，表面的污染和液体损失将不可避免。为了解决这些问题，超疏水表面上的无损液滴操作方法得到了广泛关注。
现有的无损液滴转移方法主要是基于具有可调粘附力的智能表面。通过切换高粘附力来捕获液滴，切换低粘附力来释放液滴，从而实现液滴的转移。最常用的方法是用特殊材料对表面进行处理，使表面能对外界刺激信号作出反应并改变其表面粘附特性。然而，外界刺激会降低液滴的生物活性，增加操作的复杂性。为了克服这一缺陷，也有人提出了一种通过寻找可拉伸或弯曲的柔性表面材料来运输液滴的方法。与表面改性相比，材料表面变形更方便，生物相容性更好，但表面疏水性可控范围较小，限制了其能够应用的场合。此外，上述的两种方法由于成本高，难以在工业上得到广泛应用。
因此，寻找一种可以广泛应用于各种疏水表面、且不需要外部刺激信号、廉价自由液滴转移方法是极为迫切的。
发明内容
针对现有技术中的不足，有必要提出了一种新的液滴镊子以及液滴控制方 法。
一种液滴镊子，包括：
两个镊臂；
两个疏水板，分别固定于所述两个镊臂的头端；两个所述疏水板呈角度设置；两个所述疏水板能够相对平动，且两个所述疏水板之间的角度可调。
上述液滴镊子，通过疏水不平行板结构变化可以改变液滴所受毛细管力的方向和大小，既能实现液滴的向上又能实现液滴的向下运动，从而实现了液滴的捕获/释放。不同于其他的液滴捕获/释放方法，由于这种捕获/释放液滴的力来自为不平行板本身的结构特性，所以对于不同底面的疏水性质，它表现出了广泛适用性，和优越的生物及化学的兼容性，可以成为微流体系统、液滴输送、生物分析、微反应容器等方面的强大平台。
可选地，所述疏水板包括玻璃基板以及覆在所述玻璃基板上的疏水层。
可选地，所述疏水层为特氟龙层。
可选地，所述疏水层的接触角为120度，且CAH为10度。
可选地，所述疏水层的厚度为100μm。
可选地，所述玻璃基板的厚度为150μm；所述玻璃基板的长度与宽度均为5cm。
本发明的第二个目的是，提供了一种液滴控制方法。
一种液滴控制方法，所述液滴控制方法采用本发明所提供的液滴镊子；
将所述液滴镊子靠近液滴并与液滴相接触，以形成液桥；然后减小所述液滴镊子的开合以对液滴进行捕获；
增大所述液滴镊子的夹角，然后增大所述液滴镊子的开合以对液滴进行释放。
上述液滴控制方法，采用本发明所提供的液滴镊子，通过疏水不平行板结构变化可以改变液滴所受毛细管力的方向和大小，既能实现液滴的向上又能实现液滴的向下运动，从而实现了液滴的捕获/释放。不同于其他的液滴捕获/释放方法，由于这种捕获/释放液滴的力来自为不平行板本身的结构特性，所以对于不 同底面的疏水性质，它表现出了广泛适用性，和优越的生物及化学的兼容性，可以成为微流体系统、液滴输送、生物分析、微反应容器等方面的强大平台。
优选地，在捕获过程中，在液滴镊子接触液滴前，所述液滴镊子的镊臂头端间隙L n满足以下条件：
Figure PCTCN2019116589-appb-000001
其中，α a为所述液滴镊子的界面的前进角，θ为所述液滴镊子的疏水板与垂直方向的夹角，R为液滴的球半径。
优选地，在捕获过程中，应满足以下关系：
Figure PCTCN2019116589-appb-000002
其中，H为液滴镊距底表面最小高度，L w为液滴镊子的液桥上端宽度，α a为液滴镊子的界面的前进角，β a为液滴镊子的疏水板的表面接触角，θ为所述液滴镊子的疏水板与垂直方向的夹角。
优选地，在释放过程中，增大所述液滴镊子的夹角，以至夹角大于29度。
附图说明
图1为本发明一实施例的液滴镊子的结构示意图。
图2为图1中的液滴镊子的疏水板的结构示意图。
图3为液滴捕获过程示意图。
图4为液滴释放过程示意图。
图5为在不平行板挤压/拉伸的情况下，不平行极板内液滴受力及运动趋势分析图以及实验结果图。
图6为在不平行板闭合/打开的情况下，不平行极板内液滴受力及运动趋势分析图以及实验结果图。
图7为液滴在不同
Figure PCTCN2019116589-appb-000003
和θ时的移动趋势图。
图8为液滴在不同
Figure PCTCN2019116589-appb-000004
和θ时的移动趋势图。
图9为液滴在不同
Figure PCTCN2019116589-appb-000005
和θ时的移动趋势图。
具体实施方式
为了使本发明的目的、技术方案及优点更加清楚明白，以下结合具体实施方式，对本发明进行进一步详细说明。应当理解，此处所描述的具体实施方式仅仅用以解释本发明，并不用于限定本发明。
除非另有定义，本文所使用的所有的技术和科学术语与属于本发明的技术领域的技术人员通常理解的含义相同。本文中在本发明的说明书中所使用的术语只是为了描述具体的实施方式的目的，不是旨在于限制本发明。本文所使用的术语“及/或”包括一个或多个相关的所列项目的任意的和所有的组合。
本发明的发明人发现，疏水不平行板结构的变化不仅可以改变液滴所受拉氏力的大小，而且可以改变液滴所受拉氏力的方向。
参见图5-图7，分析液滴在疏水不平行板中的受力以及运动情况。液滴运动主要受两种力的影响。第一种是由结构引起的不对称拉氏力，它引起液滴运动，决定液滴运动方向。二是接触角滞后(CAH)引起的滞后力，它阻碍液滴运动，决定液滴在拉氏力作用下能否运动。
逐一分析这两点如下：
首先，结构产生的拉氏力，这个力的大小和方向是由两个因素决定的，第一个是不平行结构中液桥底端的宽度L n，在这里，为了消除液滴大小的影响，在微尺度下，用
Figure PCTCN2019116589-appb-000006
来代替L n更精确。第二个是疏水板和垂直方向之间的角度θ。通过几何结构和拉普拉斯方程分析了这两个因素对液滴运动方向的影响。疏水不平行板模型如图5所示。假定液桥底端的接触角(CA)为α 1，上端接触角是α 2，液桥的长度是D，液桥的底端与不平行板之间的交点的距离为S，液桥中液滴的体积可以表示为：
V≈2π·D 2·(D+2S)·sinθ          (0-1)另外，根据几何关系，L n能用方程L n≈2S·sinθ来计算。由于液滴处于平衡状态，根据拉氏方程，需满足方程5-2 [42-44]：
Figure PCTCN2019116589-appb-000007
假若以特氟龙作为界面材料，构建了疏水不平行板结构，假设α 1＝α 2≈120°。根 据方程5-1和5-2，可以得到液滴运动趋势的理论曲线，如图7所示。实线为液滴压力平衡曲线，在实线以上为向下运动趋势，在实线以下为向上运动趋势。发明人发现一个更大的
Figure PCTCN2019116589-appb-000008
或θ将促进向下运动。
为了验证这一关键发现，基于表面演化理论，从三维角度模拟了液滴在疏水不平行结构中的运动趋势。从而得到了在不同
Figure PCTCN2019116589-appb-000009
和θ时的液滴运动趋势(如图7的星号符号所示)，仿真结果与理论分析是一致的(稍有不同的主要原因是由于理论分析是基于二维的)。
其次，发明人分析了CAH引起的滞后力。假设接触角的上限为前进角(下标‘a’)，下限为后退角(下标‘r’)。根据CAH的定义，当液滴向上运动时，α 1＝α r，α 2＝α a；当液滴向下移动时，α 1＝α a，α 2＝α r。由此，我们得到了液滴能克服不同CAHs，实现向上/向下运动的曲线。如图7所示，点划线/虚线为CAH＝10°时液滴向下/向上运动的临界曲线，两点线/点线为CAH＝20°时液滴向下/向上的临界曲线。然后，我们可以得到液滴在不同CAH下的运动状态。例如，由于点A(
Figure PCTCN2019116589-appb-000010
以及θ＝5°)在实线下方，液滴趋于向上运动。此外，由于点A位于点划线和两点线之间，说明当CAH≤10°时，点A仍可以向上移动，但当CAH≥20°时，点A不能向上移动。从图7中可以看出，CAH越大，对液滴运动的阻碍作用越强，但CAH对液滴运动趋势没有影响。
基于实验，
Figure PCTCN2019116589-appb-000011
和θ对于这种运动的影响也得到了验证。实验如图5a的实验部分所示，当挤压/拉伸不平行板时(平动)，也就是说减小/增加
Figure PCTCN2019116589-appb-000012
的值，会产生相应的液滴向上/向下运动；如图5b实验部分所示，当不平行板结构闭合/打开时，也就是减小/增大θ时，液滴会向上/向下移动。这些结果与理论和仿真结果完全一致。以上均表明，液滴拉氏力的方向和大小可以随着不平行板结构的变化而变化，为液滴后续的捕获/释放提供了方向。
参见图1，本发明提供了一种液滴镊子，其包括两个镊臂10、以及两个疏水板20。
其中，镊臂10的主要作用是，支撑疏水板20以及带动疏水板20运动，进而实现两个疏水板20的相互平动的开合动作，以及绕着两个疏水板20延长线 的交点旋转的开合动作。疏水板20的主要作用是，依靠两个疏水板20的相互平动的开合动作，以及绕着两个疏水板20延长线的交点旋转的开合动作，从而实现对液滴产生不同的作用力，进而实现液滴的捕获或释放。在液滴镊子捕获或释放液滴时，镊臂10并不与液滴接触，疏水板20直接与液滴接触。
具体地，两个疏水板的表面呈疏水性质。两个疏水板分别固定于两个镊臂的头端；也就是说，一个疏水板位于一个镊臂的头端，另一个疏水板位于另一个镊臂的头端。两个疏水板呈角度设置，也就是说，两个疏水板之间不平行，也即两个疏水板构成不平行板结构。两个疏水板能够相对平动，也就是说，两个疏水板能够实现相互平动的开合动作；且两个疏水板之间的角度可调，也即两个疏水板能够实现绕着两个疏水板延长线的交点旋转的开合动作。
在一优选实施方式中，参见图2，疏水板的具体结构如下：疏水板包括玻璃基板以及覆在玻璃基板上的疏水层。疏水层的作用主要是使疏水板呈现疏水性质，而玻璃基板作为基板。
在一具体实施例中，玻璃基板的厚度为150μm。玻璃基板的长度与宽度均为5cm。
在一具体实施例中，疏水层为特氟龙层。特氟龙层具有良好的疏水性能，可以进一步扩大液滴镊子的使用场合。上述疏水板可以采用如下方式制备：将玻璃片浸涂于特氟龙熔液中，然后在热板上以160度下加热固膜层30min。
在一优选实施例中，疏水层的接触角为120度，且CAH为10度。这样可以具有良好的疏水性能，也可以进一步扩大液滴镊子的使用场合。
更进一步地，疏水层的厚度优选为100μm。
当然可以理解的是，本发明并不局限于玻璃基板，亦可以采用其它材料作为基板。同样地，疏水层也并不局限于特氟龙层，亦可以是其它材料制成的疏水层。进一步还可以理解的是，疏水板亦可以是一体式的，也即直接用疏水材料制成疏水板，或者基板的表面微观结构直接使其表面疏水化。
本发明还提供了一种液滴控制方法。
一种液滴控制方法，所述液滴控制方法采用本发明所提供的液滴镊子；
将所述液滴镊子靠近液滴并与液滴相接触，以形成液桥；然后减小所述液滴镊子的开合以对液滴进行捕获；
增大所述液滴镊子的夹角，然后增大所述液滴镊子的开合以对液滴进行释放。
以下对捕获过程进行分析：
首先，液滴镊子垂直向下接近液滴，然后液滴部分进入液镊形成一个液桥(如图3a-b)。第二，继续向下移动液滴镊子将更多滴液挤入镊子，这也意味着减少
Figure PCTCN2019116589-appb-000013
(如图3的b-c)。第三，通过挤压，液滴与底面接触面积减小，粘合力减小。此外，这种挤压也降低了
Figure PCTCN2019116589-appb-000014
的值，这就增加了向上的毛细管力。然后，产生了液滴的向上运动(图3的c-d)。最后，通过继续挤压液滴，可以使液滴完全进入液滴镊子中(图3的d-e)。
发明人发现在液滴捕获过程中有四个可控变量；在第一步中的初始液滴镊子尖端宽度(L Ini，也就是L n的初始值)和关键的不平行板间夹角(θ)；第二步中的液滴镊子的最终下压高度(H)；第三步中液滴尖端的最终宽度(L Final，L n的最终值)。然后，下面几段将分别讨论这四个变量。
1、选择适当的初始液滴镊子尖端宽度L Ini和角度θ，确保水滴能部分进入液滴镊子中(第一步)
在初始状态下，液滴镊子内没有液体。随着液滴镊子向下运动，液滴将进入液滴镊子内。但如果初始液滴镊头尖端过小，液滴会被挤压到液滴镊子的一侧。为了避免这种情况，最初的接触角α需要满足α＞α a(α a为液面前进角)。然后，结合几何关系，可以得到关于L Ini和θ的条件方程，液滴可以部分进入疏水不平行板结构：
Figure PCTCN2019116589-appb-000015
式中，R为开放表面上液滴的球形半径，L Ini为初始液滴镊子的尖端宽度。根据方程5-3，发现L Ini和R是线性相关的。而R是由液滴体积大小
Figure PCTCN2019116589-appb-000016
和底面的湿润性决定的。因此，如果假设底部板是由Teflon(β a＝120°)覆盖，然后可以计算出在不同θ时，液滴进入液滴镊子的
Figure PCTCN2019116589-appb-000017
的取值范围。对三种不同的组 合的
Figure PCTCN2019116589-appb-000018
和θ进行了实验，发现液滴能进入液体镊子，这与理论分析是一致的。
2、合适的液镊最终下压高度H(第二步和第三步)
第二步是必然发生的，所以对于控制参数没有要求。从理论角度对这个结论进行了说明，定义在液镊内的部分为Part 1，其中的压力为P 1；液镊下的部分为Part 2，其中的压力为P 2。所以，P 1和P 2能用下面的方程计算：
Figure PCTCN2019116589-appb-000019
Figure PCTCN2019116589-appb-000020
式中，L w为液滴镊液桥上端宽度，H为液滴镊距底表面高度。当液滴镊垂直向下运动时(H减小)，也就是挤压Part 2时，P 2增大。同时，随着液滴进入液滴镊内，Part 1中的液滴增大，L w增大，P 1减小。可以看出，液桥形成后，在液滴镊向下运动的过程中，Part 1和Part 2(ΔP＝P 2-P 1)的压差增大，液滴不可避免地会向上液滴镊的方向移动。
H主要受到第三步的限制。如果需要将液滴与底面分离，则应克服粘附力。为了减少这种粘附力，挤压液滴以减少接触面积，也就是减少底部表面的接触线长度。为了完成这一步，应该避免泄漏。那么，液滴是否泄漏取决于两个条件：第一，如果Part 1的运动趋势是向上的，则不会泄漏；第二，如果Part 1有向下移动的趋势，那么底部表面的“液阀”是否可以防止这种泄漏。对于第一个条件，根据上面对于Part 1的分析和方程L w≈2(S+D)·sinθ，可以得到向下运动时的
Figure PCTCN2019116589-appb-000021
的取值范围。对于第二个条件，那么必须满足β＜β a。由式(5-4)、(5-5)可得能有效防止泄漏的H约束条件：
Figure PCTCN2019116589-appb-000022
另外，对
Figure PCTCN2019116589-appb-000023
和
Figure PCTCN2019116589-appb-000024
关系进行了分析。假设液滴位于Teflon表面，它的前进角是120度，它的初始半径为R，所以其体积
Figure PCTCN2019116589-appb-000025
假设在液滴镊子被挤压之前，液滴高度为H，液滴的Part 2近似为圆柱体。因此，液滴的体积可以近似为
Figure PCTCN2019116589-appb-000026
因为L n＜2R，所以V part2≤πHR 2，并且
Figure PCTCN2019116589-appb-000027
从而我们得到了
Figure PCTCN2019116589-appb-000028
和
Figure PCTCN2019116589-appb-000029
的近似变换关系，进而得到了
Figure PCTCN2019116589-appb-000030
的取值范围。
根据上述两个条件，结合对于
Figure PCTCN2019116589-appb-000031
和
Figure PCTCN2019116589-appb-000032
关系的分析，得到了在不同θ的情况下的
Figure PCTCN2019116589-appb-000033
的取值范围。如图8所示，实线上方表示可能发生泄露，下方表示不会泄露。为了验证这个结论，对于不同
Figure PCTCN2019116589-appb-000034
和θ时的情况进行了实验验证。从图中可知，实验结果和理论相一致。
3、能在第三步中成功捕获液滴的液滴镊子的最终尖端宽度范围(L Final)
在第三步中需要L Final的值较小。如果Part 1的液滴能够克服CAH的阻力，在挤压后向上运动，则会使液滴远离底板(此时，由于底面接触面积小，附着力小，V part1≈V)。因此，根据之前分析，可以获得当在不同θ时，液滴可以克服CAH和并完全进入到液滴镊子的
Figure PCTCN2019116589-appb-000035
的范围(图9中的实线下的部分)。通过测量不同θ情况下，液滴完全进入液滴镊子时的
Figure PCTCN2019116589-appb-000036
的值来证实这个理论结果(图9中的米子标记点位)。发现这些点在实线以下，实验结果与理论分析吻合较好。
以下对释放过程进行分析。
首先，通过旋转轴增加θ，液滴运动趋势将从向上变为向下。第二，通过释放滴镊子，增加
Figure PCTCN2019116589-appb-000037
同样增加向下的毛细管力(图4中的f-g)。第三，毛细管力将克服CAH的阻力和自发向下运动，液滴完全集中在疏水不平行板底部(图4中的g-i)。最后，通过微小的放松，液滴将掉落到超疏水表面，实现液滴的成功释放(图4中的i-j)。分析这个过程，发现其中只有一个可控制的量，那就是，在垂直方向，在释放过程中。发现在整个过程中，只有一个可控的量θ，也就是液滴镊子和垂直方向之间的角度。
根据前面分析，随着θ的增加，毛细管力将由向上变为向下并不断变大，这为液滴的向下运动提供动力。根据图7所示，发现，当θ＞29°，液滴运动趋势必然会表现出下降的趋势，否则，它可能会有上升趋势。然而，这种向上的运动使液滴粘附在液滴镊子的一侧，而不是脱落。因此，可以确定成功释放液滴的θ的范围(θ＞29°)。
此外，为了防止液滴粘附到液滴镊子的底面，需要保证液滴镊子的底面足够窄，且侧面相对疏水。优选100μm厚度和特氟龙覆盖的液滴镊子，可确保液滴 在大于0.8微升时可以通过重力掉落。
优选地，在捕获过程中，在液滴镊子接触液滴前，所述液滴镊子的镊臂头端间隙L n满足以下条件：
Figure PCTCN2019116589-appb-000038
其中，α a为所述液滴镊子的界面的前进角，θ为所述液滴镊子的疏水板与垂直方向的夹角，R为液滴的球半径。
在捕获过程中，应满足以下关系：
Figure PCTCN2019116589-appb-000039
其中，H为液滴镊距底表面最小高度，L w为液滴镊子的液桥上端宽度，α a为液滴镊子的界面的前进角，β a为液滴镊子的疏水板的表面接触角，θ为所述液滴镊子的疏水板与垂直方向的夹角。
优选地，在释放过程中，增大所述液滴镊子的夹角，以至夹角大于29度。
以下对本发明液滴镊子对液滴的捕获或释放方法的阐述。
液滴镊子在疏水面捕获和在超疏水面上释放液滴过程如图3、图4所示。
捕获过程：首先根据液滴大小选择合适的液滴镊子初始间隙，将液滴镊子垂直向下(图3-a)，使两个疏水板靠近液滴并与液滴相接触，从而使得两个疏水板中形成液桥(图3-b)；之后，选择合适的液滴镊子下压高度，继续向下移动两个疏水板使液滴能更多的进入两个疏水板之间(图3-c)；然后，选择合适的液滴镊子挤压距离，通过两个疏水板两侧的向内挤压减少液滴与底面的接触从而减少粘附力(adhesion force)并且同时也减小了而获得更大的向上的毛细管力(图3-d)，最后，通过继续挤压液滴能完全进入不平行板之间，完成液滴的捕获(图3-e)。
释放过程：选择合适的液滴镊子的夹角，通过增加液滴镊子的夹角(图4-f)，液滴运动趋势会由向上变为向下，液滴向下运动(图4-g)；之后，选择合适的液滴镊子的顶端间隙，通过增加液滴镊子的疏水板的间距，通过增加进一步增加向下的毛细管力(图4-h)，之后液滴由于较大的毛细管力会克服了其CAH的阻力自发向下运动(图4-i)，液滴完全集中于液滴镊子的底部，通过微小的 一个放松动作(relaxing)，液滴就会下落于超疏水表面上(图4-j)从而成功实现液滴的释放。
上述液滴镊子，通过疏水不平行板结构变化可以改变液滴所受毛细管力的方向和大小，既能实现液滴的向上又能实现液滴的向下运动，从而实现了液滴的捕获/释放。不同于其他的液滴捕获/释放方法，由于这种捕获/释放液滴的力来自为不平行板本身的结构特性，所以对于不同底面的疏水性质，它表现出了广泛适用性，和优越的生物及化学的兼容性，可以成为微流体系统、液滴输送、生物分析、微反应容器等方面的强大平台。
本发明还提供了一种液滴捕获释放装置。
一种液滴捕获释放装置，包括：
液滴镊子，为本发明所提供的液滴镊子；
平动机构，连接在所述液滴镊子的镊臂的尾端且控制所述镊臂平动开合；
以及旋转机构，连接在所述镊臂的尾端且控制所述镊臂旋转开合。
其中，平动机构的主要作用是，控制镊臂相互平动的开合动作，进而实现疏水板相互平动的开合动作。旋转机构的主要作用是，控制镊臂相对旋转的开合动作，进而实现两个疏水板绕着两个疏水板延长线的交点旋转的开合动作。。
在一具体实施例中，平动机构为微型电动夹。微型电动夹的精度控制可以为0.2微米，控制更精确。
更进一步地，液滴捕获释放装置还包括XYZ三轴控制平台，微型电动夹安装在XYZ三轴控制平台上。XYZ三轴控制平台实现液滴捕获及释放过程的定位；其中，通过XY控制液滴在底面上的位置(其精度优选控制为0.2微米)，通过z轴来控制液滴镊子捕获液滴时的液滴镊子高度(其精度优选控制为0.2微米)。
参见图1，可选地，镊臂10的末端设有旋转腰形孔11。这样可以有利于控制疏水板绕着两个疏水板延长线的交点旋转的开合动作。优选地，精度优选控制为1°。
上述液滴捕获释放装置，采用本发明所提供的液滴镊子，通过疏水不平行板结构变化可以改变液滴所受毛细管力的方向和大小，既能实现液滴的向上又能 实现液滴的向下运动，从而实现了液滴的捕获/释放。不同于其他的液滴捕获/释放方法，由于这种捕获/释放液滴的力来自为不平行板本身的结构特性，所以对于不同底面的疏水性质，它表现出了广泛适用性，可以成为微流体系统、液滴输送、生物分析、微反应容器等方面的强大平台。
以上所述实施例的各技术特征可以进行任意的组合，为使描述简洁，未对上述实施例中的各个技术特征所有可能的组合都进行描述，然而，只要这些技术特征的组合不存在矛盾，都应当认为是本说明书记载的范围。
以上所述实施例仅表达了本发明的几种实施方式，其描述较为具体和详细，但并不能因此而理解为对发明专利范围的限制。应当指出的是，对于本领域的普通技术人员来说，在不脱离本发明构思的前提下，还可以做出若干变形和改进，这些都属于本发明的保护范围。因此，本发明专利的保护范围应以所附权利要求为准。

Claims (10)

  1. 一种液滴镊子，其特征在于，包括：
    两个镊臂；
    两个疏水板，分别固定于所述两个镊臂的头端；两个所述疏水板呈一定范围的角度设置；两个所述疏水板能够相对平动，且两个所述疏水板之间的角度可调。
  2. 根据权利要求1所述的液滴镊子，其特征在于，所述疏水板包括玻璃基板以及覆在所述玻璃基板上的疏水层。
  3. 根据权利要求2所述的液滴镊子，其特征在于，所述疏水层为特氟龙层。
  4. 根据权利要求2所述的液滴镊子，其特征在于，所述疏水层的接触角为120度，且接触角滞后(CAH)为10度。
  5. 根据权利要求2所述的液滴镊子，其特征在于，所述疏水层的厚度为100nm。
  6. 根据权利要求2所述的液滴镊子，其特征在于，所述玻璃基板的厚度为150μm。
  7. 一种液滴控制方法，其特征在于，所述液滴控制方法采用权利要求1-6任一项所述的液滴镊子；
    将所述液滴镊子靠近液滴并与液滴相接触，以形成液桥；然后减小所述液滴镊子的开合以对液滴进行捕获；
    增大所述液滴镊子的夹角，然后增大所述液滴镊子的开合以对液滴进行释放。
  8. 根据权利要求7所述的液滴控制方法，其特征在于，在捕获过程中，在液滴镊子接触液滴前，所述液滴镊子的镊臂头端间隙L n满足以下条件：
    Figure PCTCN2019116589-appb-100001
    其中，α a为所述液滴镊子的界面的前进角，θ为所述液滴镊子的疏水板与垂直方向的夹角，R为液滴的球半径。
  9. 根据权利要求7所述的液滴控制方法，其特征在于，在捕获过程中，应满足以下关系：
    Figure PCTCN2019116589-appb-100002
    其中，H为液滴镊距底表面最小高度，L w为液滴镊子的液桥上端宽度，α a为液滴镊子的界面的前进角，β a为液滴镊子的疏水板的表面接触角，θ为所述液滴镊子的疏水板与垂直方向的夹角。
  10. 根据权利要求7所述的液滴控制方法，其特征在于，在释放过程中，增大所述液滴镊子的夹角，以至夹角大于29度。
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