静电纺丝过程行为及振动静电纺丝技术研究
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摘要
静电纺丝技术可以生产纳米纤维并且其生产过程简单而又经济，因此该技术已经引起了世界范围内的广泛关注，静电纺丝技术的研究工作在广泛的开展之中。但是静电纺丝技术中仍存在一些难以解决的问题，还有很多技术和理论工作需要进一步的深入和完善。
本文构造了静电纺丝过程的一维定常模型，并且考虑到静电纺丝中的热、电效应，得到了改进的Spivak-Dzenis模型和一维静电纺丝模型，对静电纺丝技术进行了理论性的描述，所得的模型相对以往的模型更为完善，对静电纺丝技术的研究具有更强的指导性。
本文突破了描述单一阶段的Spivak关于射流直径与射流运行距离之间的关系式，得到了不同阶段射流直径与射流运动距离之间的关系式。Spivak关系式已被学术界普遍接受并广泛引用，但是通过对静电纺丝过程中不稳定现象的分析研究，本文认为这一关系式具有一定的局限性，只适用于射流运动过程中的某一阶段，通过对本文所建立模型的分析，本文最终得到了分别对应射流运动中的初始阶段、不稳定阶段和最终阶段的射流直径与射流运动距离之间的关系式，与Spivak的关系式相比，这些关系式更具有普遍适用性与指导意义。
本文引入标度率分析方法，建立了电流与电压、纤维直径与电压、电流与流量、纤维直径与流量等主要参数之间的标度率关系式，并进行了实验验证。利用这些关系式可以指导静电纺丝工艺的生产和控制，并可以实现对纳米纤维直径的预测，具有重要的实验和生产指导意义。
本文突破以往静电纺丝装置的研究开发方向，通过理论分析和实验验证证实了振动静电纺丝技术的可行性并自主开发了振动静电纺丝装置。在一般静电纺丝装置中存在纺丝困难的高浓度溶液，利用该设备可以顺利纺丝，并可以获得直径更细的纤维。
本文利用自主研发的振动静电纺丝装置对若干溶液体系进行了应用研究，考察了振动静电纺丝装置的应用方向和应用前景。在振动静电纺丝实验过程中，不具有流动性的聚氧乙烯凝胶体系呈现了良好的流动性和可纺性，并最终获得了平均直径为100纳米的聚氧乙烯纳米纤维。在对可纺性不强的聚丁二酸丁二醇酯溶液进行的振动静电纺丝实验中，聚丁二酸丁二醇酯溶液呈现了良好的可纺性，纺丝实验非常顺利，与使用普通静电纺丝装置获得的聚丁二酸丁二醇酯纤维相比，使用振动静电纺丝装置纺出的聚丁二酸丁二醇酯纤维直径显著变细了。对添加了未特殊处理碳纳米管的聚丙烯腈溶液的振动电纺丝中，获得了碳纳米管分布均匀、取向良好的碳纳米管增强的聚丙烯腈纤维。这些实验的成功，证明振动静电纺丝技术提高溶液的可纺性，实现对普通静电纺丝装置纺丝存在困难的溶液体系的正常纺丝，并可以得到直径更细的纤维；同时对含有纳米颗粒的高聚物溶液体系的振动静电纺丝，则可以获得颗粒分散均匀、取向良好的纳米纤维。因此，振动静电纺丝技术在静电纺丝溶液体系趋于多样化的情况下具有广泛的可用性和良好的发展前景。
Electrospinning technology has obtained word-wide attention for its convenience in producing nanofibers. Electrospinning is a technology using electric force supplied by a high voltage field to eject Taylor Cone into jets which are finally dried and solidified into nano-scale fibers as solvents vaporized. Mathematical model is a key point for development of electrospinning technology. Though much research has been conducted experimentally and theoretically, its mathematical model is far from perfect possibly due to the complex and nonlinear phenomena and quantum-like properties involved in the proposes, and many factors affecting the procedure such as solutions or melts' viscosity, molecular weight, entanglement of the macromolecule, applied voltage, flow rate and ambience. Based on known models (e.g. Spivak-Dzenis model), a more complete mathematical model is established considering more effects on the procedure, which has wide applications. Its reduced one-dimensional model is of utter simplicity, and has many practical applications.
Diameter is a key parameter of electrospun nanofiber, which determines whether the obtained fiber could have magic nano-effect properties. Much attention was paid on the prediction. of diameter of electrospun nanofiber. Spivak suggested a ubiquitous scaling law between the jet diameter and its running distance which was widely used. Through analysis of different stages in the procedure of electrospinning, we find the scaling law is valid only for a special stage. Based on our established mathematical model, we obtain different scaling laws for different stages in the procedure. Also we obtain various scaling laws which can not be obtained by other models, such as the relationships between voltage and solution flow rate, diameter of the obtained fiber and voltage, current and voltage, diameter and flow rate, and others. All these scalings are experimentally verified and have many potential applications in experiment.
Experiments and theoretical analysis reveal that polymer solution Can not be electrospun into nanofibers when the Solution viscosity surpasses a certain threshold. We designed a new set of electrospinning set-up coupled with ultrasonic equipment. Some experiments were carried with the new set-up and experimental results showed that our novel vibration-electrospinning apparatus can produce nanofibers from those solutions with high viscosity or coagulated which can not be ecletrospun by classical electrospinning processes; and also the apparatus leads to much finer nanofibers than those obtained without vibration. Furthermore, eletrospinning of original carbon nanotubes added in polymer solution shows that our vibration-electrospinning apparatus works well on additives enhanced nanofibers with good dispersion and alignment.
本文构造了静电纺丝过程的一维定常模型，并且考虑到静电纺丝中的热、电效应，得到了改进的Spivak-Dzenis模型和一维静电纺丝模型，对静电纺丝技术进行了理论性的描述，所得的模型相对以往的模型更为完善，对静电纺丝技术的研究具有更强的指导性。
本文突破了描述单一阶段的Spivak关于射流直径与射流运行距离之间的关系式，得到了不同阶段射流直径与射流运动距离之间的关系式。Spivak关系式已被学术界普遍接受并广泛引用，但是通过对静电纺丝过程中不稳定现象的分析研究，本文认为这一关系式具有一定的局限性，只适用于射流运动过程中的某一阶段，通过对本文所建立模型的分析，本文最终得到了分别对应射流运动中的初始阶段、不稳定阶段和最终阶段的射流直径与射流运动距离之间的关系式，与Spivak的关系式相比，这些关系式更具有普遍适用性与指导意义。
本文引入标度率分析方法，建立了电流与电压、纤维直径与电压、电流与流量、纤维直径与流量等主要参数之间的标度率关系式，并进行了实验验证。利用这些关系式可以指导静电纺丝工艺的生产和控制，并可以实现对纳米纤维直径的预测，具有重要的实验和生产指导意义。
本文突破以往静电纺丝装置的研究开发方向，通过理论分析和实验验证证实了振动静电纺丝技术的可行性并自主开发了振动静电纺丝装置。在一般静电纺丝装置中存在纺丝困难的高浓度溶液，利用该设备可以顺利纺丝，并可以获得直径更细的纤维。
本文利用自主研发的振动静电纺丝装置对若干溶液体系进行了应用研究，考察了振动静电纺丝装置的应用方向和应用前景。在振动静电纺丝实验过程中，不具有流动性的聚氧乙烯凝胶体系呈现了良好的流动性和可纺性，并最终获得了平均直径为100纳米的聚氧乙烯纳米纤维。在对可纺性不强的聚丁二酸丁二醇酯溶液进行的振动静电纺丝实验中，聚丁二酸丁二醇酯溶液呈现了良好的可纺性，纺丝实验非常顺利，与使用普通静电纺丝装置获得的聚丁二酸丁二醇酯纤维相比，使用振动静电纺丝装置纺出的聚丁二酸丁二醇酯纤维直径显著变细了。对添加了未特殊处理碳纳米管的聚丙烯腈溶液的振动电纺丝中，获得了碳纳米管分布均匀、取向良好的碳纳米管增强的聚丙烯腈纤维。这些实验的成功，证明振动静电纺丝技术提高溶液的可纺性，实现对普通静电纺丝装置纺丝存在困难的溶液体系的正常纺丝，并可以得到直径更细的纤维；同时对含有纳米颗粒的高聚物溶液体系的振动静电纺丝，则可以获得颗粒分散均匀、取向良好的纳米纤维。因此，振动静电纺丝技术在静电纺丝溶液体系趋于多样化的情况下具有广泛的可用性和良好的发展前景。
Electrospinning technology has obtained word-wide attention for its convenience in producing nanofibers. Electrospinning is a technology using electric force supplied by a high voltage field to eject Taylor Cone into jets which are finally dried and solidified into nano-scale fibers as solvents vaporized. Mathematical model is a key point for development of electrospinning technology. Though much research has been conducted experimentally and theoretically, its mathematical model is far from perfect possibly due to the complex and nonlinear phenomena and quantum-like properties involved in the proposes, and many factors affecting the procedure such as solutions or melts' viscosity, molecular weight, entanglement of the macromolecule, applied voltage, flow rate and ambience. Based on known models (e.g. Spivak-Dzenis model), a more complete mathematical model is established considering more effects on the procedure, which has wide applications. Its reduced one-dimensional model is of utter simplicity, and has many practical applications.
Diameter is a key parameter of electrospun nanofiber, which determines whether the obtained fiber could have magic nano-effect properties. Much attention was paid on the prediction. of diameter of electrospun nanofiber. Spivak suggested a ubiquitous scaling law between the jet diameter and its running distance which was widely used. Through analysis of different stages in the procedure of electrospinning, we find the scaling law is valid only for a special stage. Based on our established mathematical model, we obtain different scaling laws for different stages in the procedure. Also we obtain various scaling laws which can not be obtained by other models, such as the relationships between voltage and solution flow rate, diameter of the obtained fiber and voltage, current and voltage, diameter and flow rate, and others. All these scalings are experimentally verified and have many potential applications in experiment.
Experiments and theoretical analysis reveal that polymer solution Can not be electrospun into nanofibers when the Solution viscosity surpasses a certain threshold. We designed a new set of electrospinning set-up coupled with ultrasonic equipment. Some experiments were carried with the new set-up and experimental results showed that our novel vibration-electrospinning apparatus can produce nanofibers from those solutions with high viscosity or coagulated which can not be ecletrospun by classical electrospinning processes; and also the apparatus leads to much finer nanofibers than those obtained without vibration. Furthermore, eletrospinning of original carbon nanotubes added in polymer solution shows that our vibration-electrospinning apparatus works well on additives enhanced nanofibers with good dispersion and alignment.
引文
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