Advancing Materials Discovery and Electronics Fabrication via Aerosol Jet Printing

Aerosol jet printing (AJP) is a versatile additive manufacturing (AM) method that can deposit a wide range of organic and inorganic materials with high spatial resolution of about 10 µm. Over the past decade, AJP has been extensively applied to fabricate electronics, sensors, and energy conversion and storage devices. However, numerous potential fields remain unexplored. This thesis presents a novel aerosol-based high-throughput combinatorial printing (HTCP) method to accelerate materials discovery and a non-thermal plasma-integrated AJP to print electronics on temperature-sensitive substrates such as textiles, plants, and hydrogels. For the applications of high-throughput materials discovery, the unique combinatorial AJP system realizes in situ mixing of multiple aerosolized inks and fast modulation of the mixing ratio on-the-fly during the printing process. Consequently, combinatorial materials with compositional gradients at microscale spatial resolution were achieved. A series of high-throughput printing strategies and applications, including combinatorial doping and functional grading, were demonstrated. A functionally graded polymer-based solid-state electrolyte with gradient compositions along the film thickness direction was prepared. The electrolyte delivers enhanced energy storage performance when used in the high voltage lithium metal batteries. For the applications of printing electronics on temperature-sensitive substrates, non-thermal plasma was introduced to the AJP system. The plasma jet can convert aerosolized inks into highly conductive metal patterns at room temperature without damaging the temperature-sensitive substrates. This method was first applied to the fabrication of gold electrodes on permeable textiles for human health monitoring. As a demonstration, glucose and hydrogen peroxide sensors were fabricated on nylon fabric for human health monitoring. Then, the plasma integrated AJP was used to print gold electrodes on leaves with barbed surface for plant health monitoring. Lastly, this method was employed to pattern bioelectronics on hydrogels. The use of in situ plasma treatment produced electrodes with high conductivity, strong bonding, and excellent stretchability.气溶胶喷射打印（Aerosol Jet Printing, AJP）是一种通用型增材制造（Additive Manufacturing, AM）技术，可沉积多种有机与无机材料，空间分辨率可达约10微米。近十年来，AJP已被广泛应用于电子器件、传感器以及能量转换与存储装置的制备，但仍有众多潜在应用领域尚未被探索。本论文提出了一种新型基于气溶胶的高通量组合式打印（High-Throughput Combinatorial Printing, HTCP）方法以加速材料研发，同时开发了集成非热等离子体的AJP技术，可在纺织品、植物及水凝胶等温度敏感基底上打印电子器件。 针对高通量材料研发场景，这套独特的组合式AJP系统可实现多种气溶胶化墨水的原位混合，并在打印过程中实时快速调节混合比例。最终，在微尺度空间分辨率下制备出了具有成分梯度的组合式材料。本研究验证了一系列高通量打印策略及其应用，包括组合掺杂与功能梯度调控。我们制备了一种沿膜厚方向具备成分梯度的功能梯度聚合物基固态电解质，将其应用于高压锂金属电池时，可显著提升储能性能。 针对温度敏感基底上的电子打印应用，本研究将非热等离子体引入AJP系统。等离子体射流可在室温条件下将气溶胶化墨水转化为高导电金属图案，且不会损伤温度敏感基底。该方法首先被用于在透水纺织品上制备金电极，用于人体健康监测。作为演示案例，我们在尼龙织物上制备了葡萄糖与过氧化氢传感器，用于人体健康监测。随后，集成等离子体的AJP技术被用于在带倒刺表面的叶片上打印金电极，以监测植物健康。最后，该方法被用于在水凝胶上制备生物电子器件图案。通过原位等离子体处理得到的电极具备高导电性、强附着力以及优异的拉伸性能。