Microfluidic tools and techniques for manipulating fluid droplets have become core to many scientific and technological fields. Despite the plethora of existing approaches to fluidic manipulation, non-Newtonian fluid phenomena are rarely taken advantage of. Here we introduce embedded droplet printing—a system and methods for the generation, trapping, and processing of fluid droplets within yield-stress fluids, materials that exhibit extreme shear thinning. This technique allows for the manipulation of droplets under conditions that are simply unattainable with conventional microfluidic methods, namely the elimination of exterior influences including convection and solid boundaries. Because of this, we believe embedded droplet printing approaches an ideal for the experimentation, processing, or observation of many samples in an “absolutely quiescent” state, while also removing some troublesome aspects of microfluidics including the use of surfactants and the complexity of device manufacturing. We characterize a model material system to understand the process of droplet generation inside yield-stress fluids and develop a nascent set of archetypal operations that can be performed with embedded droplet printing. With these principles and tools, we demonstrate the benefits and versatility of our method, applying it toward the diverse applications of pharmaceutical crystallization, microbatch chemical reactions, and biological assays.
We present a paradigm for the design of yield-stress fluids, using six archetypal materials for demonstration. By applying concepts of engineering design, we outline a materials design paradigm that includes (i) morphological organization based on jammed versus networked microstructures, (ii) collected scaling laws for predictive design, (iii) low-dimensional descriptions of function-valued flow data, (iv) consideration of secondary properties including viscous behavior, and (v) a strategy for material concept synthesis based on the juxtaposition of microstructures. By explicitly specifying these design strategies, we seek to create an ontology and database for the engineering of yield-stress fluids. Our proposed design strategy increases the likelihood of finding an optimal material and prevents design fixation by considering multiple material classes to achieve a desired rheological performance. This flips the typical structure-to-rheology analysis to become the inverse: rheology-to-structure with multiple possible materials as solutions.
Reversible transformations in bulk polymers offer numerous possibilities for materials remodeling and reprocessing. While reversible systems based on dynamic covalent chemistry such as the Diels–Alder reaction and transesterification have been intensively studied to enable local bond dissociation and formation, reports regarding the reversion from bulk network polymers to monomers are rare. Herein, we report a reversibly polymerizable system based on ring-opening metathesis polymerization of cyclopentene derivatives in the bulk state. The network polymer is thermodynamically stable and mechanically robust at room temperature and readily depolymerizes at elevated temperatures to yield liquid monomers that are repolymerized to cross-linked polymers by simply cooling to room temperature. This reversible process was characterized by differential scanning calorimetry and rheological tests.
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