TiO2 is an important material widely used in optoelectronic devices due to its semiconducting and photocatalytic properties, nontoxicity, and chemically inert nature. Some indicative applications include water purification systems and energy harvesting. The use of solution, water-based inks for the direct writing of TiO2 on flexible substrates is of paramount importance since it enables low-cost and low-energy intensive large-area manufacturing, compatible with roll-to-roll processing. In this work we study the effect of crystalline TiO2 and polymer addition on the rheological and direct writing properties of Ti-organic/TiO2 inks. We also report on the bridging crystallite formation from the Ti-organic precursor into the TiO2 crystalline phase, under ultraviolet (UV) exposure or mild heat treatments up to 150 °C. Such crystallite formation is found to be enhanced by polymers with strong polarity and pKα such as polyacrylic acid (PAA). X-ray diffraction (XRD) coupled with Raman and X-ray photoelectron (XPS) spectroscopy are used to investigate the crystalline-phase transformation dependence based on the initial TiO2 crystalline-phase concentration and polymer addition. Transmission electron microscopy imaging and selected area electron diffraction patterns confirm the crystalline nature of such bridging printed structures. The obtained inks are patterned on flexible substrates using nozzle-based robotic deposition, a lithography-free, additive manufacturing technique that allows the direct writing of material in specific, digitally predefined, substrate locations. Photocatalytic degradation of methylene blue solutions highlights the potential of the studied films for chemical degradation applications, from low-cost environmentally friendly materials systems.
In this work, coaxial conductor–ceramic direct ink writing enables the printing of sensitive or encapsulated materials onto heterogeneous and rough substrates. While encasing the core fluid within a stiff ceramic shell, continuity may be maintained, even while printing onto conventionally challenging substrates. Here, we report the development of a coaxial ceramic direct ink writing suite and explore coflow interrelationships based on microfluidic principles. A coaxial nozzle is designed to facilitate the coextrusion of an alumina shell, whereas indium–tin-oxide inks constitute the core. In this manner, a core–shell ceramic element may be printed onto rough substrates for future high-temperature applications. Colloidal inks are engineered to provide the required rheological and sintering performance. Moreover, flow simulations in conjunction with microfluidic coflow principles are used to explore the coaxial printing processing space, thus controlling the core–shell architectures. Physical modeling is further used to analyze core deformations and eccentricity. Simulations are validated experimentally, and the analyses are used to deposit coaxial ceramic features onto heterogeneous, high-temperature ceramic substrates.
Flexible electronics manufacturing from functional inks is a versatile approach gaining interest from both industry and academia at an accelerated pace; towards its full development, research studies establishing connections between the inks processing conditions and final materials functionalities become necessary. In this work, we report on the relations between synthesis, continuous - flow direct writing parameters, and low energy intensity post-processing of functional TiO2 hybrid ink patterns. Such inks are printed on heat sensitive polymer substrates with typical application in dye solar cell photoelectrodes; nevertheless, their versatility spans a wide range of other applications from sensors to photocatalysts. For the ink formulation, we use an initial crystalline nanoparticle TiO2 phase that provides the main functionality of the printed films. We also add a Ti-precursor that, when post-treated, provides connecting paths for the initial phase thus forming continuous porous structures. We find that the ink’s formulation plays a pivotal role by providing the means for tuning its rheological properties (necessary for successful direct writing), the ink-substrate interactions, and the printed microstructures. We further discuss the implications of such compositional variations, introduced when adding polymeric agents, such as polyacrylic acid, on the crystallization of the Ti-organic precursor into TiO2 bridges between the nanoparticles. We finally report on the electrical properties of the printed TiO2 photoelectrodes as compared to conventionally fabricated counterparts. The design, continuous – flow direct writing, and the subsequent mild thermal-energy treatments of hybrid sol-gel based TiO2 inks may hold the key for large-scale and sustainable additive manufacturing of flexible functional components for a range of applications.
Solid-State Lithium Ion Batteries are the future of lithium ion energy storage technology, showing increased theoretical capacity and safety compared to their liquid electrolyte counterparts. However, poor mechanical contact and high resistance at the electrode-electrolyte junction prevent their wider adaptation. Direct Ink Writing (DIW) is an effective tool for electrode printing due to its ability to quickly and uniformly fabricate high surface area patterns and complex microstructures, increasing interfacial contact with a polymer electrolyte and boosting performance. This project will focus on creating, testing, and optimizing cathodes designed for Solid-State Lithium Ion batteries consisting of LFP (LiFePO4) based ink directly printed onto an aluminum current collector. The project goal is to optimize the rheology of the ink, particle loading, and patterning which will result in cathodes with improved electrochemical performance while maintaining mechanical durability in a quick and reliable manner. As such, various three-dimensional microlattice patterns and particle loadings will be tested to determine which combination results in the best cathode. DIW of electrodes for solid-state batteries may hold the key for the development and manufacture of the next generation of energy storage devices, greatly impacting our ability to utilize and further adopt renewable energy sources.
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