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Free, publicly-accessible full text available August 1, 2026
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Free, publicly-accessible full text available June 11, 2026
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This article presents the first use of shape forming elements (SFEs) to produce architected composites from multiple materials in an extrusion process. Each SFE contains a matrix of flow channels connecting input and output ports, where materials are routed between corresponding ports. The mathematical operations of rotation and shifting are described, and design automation is explored using Bayesian optimization and genetic algorithms to select fifty or more parameters for minimizing two objective functions. The first objective aims to match a target cross-section by minimizing the pixel-by-pixel error, which is weighted with the structural similarity index (SSIM). The second objective seeks to maximize information content by minimizing the SSIM relative to a white image. Satisfactory designs are achieved with better objective function values observed in rectangular rather than square flow channels. Validation extrusion of modeling clay demonstrates that while SFEs impose complex material transformations, they do not achieve the material distributions predicted by the digital model. Using the SSIM for results comparison, initial stages yielded SSIM values near 0.8 between design and simulation, indicating a good initial match. However, the control of material processing tended to decline with successive SFE processing with the SSIM of the extruded output dropping to 0.023 relative to the design intent. Flow simulations more closely replicated the observed structures with SSIM values around 0.4 but also failed to predict the intended cross-sections. The evaluation highlights the need for advanced modeling techniques to enhance the predictive accuracy and functionality of SFEs for biomedical, energy storage, and structural applications.more » « less
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Free, publicly-accessible full text available January 17, 2026
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The halogen-free synthesis of oligosilazanes has been observed upon dehydrocoupling silanes with ammonia at 25 °C using [(2,6-iPr2PhBDI)Mn(µ-H)]2. Extending this methodology to polymethyl-hydrosiloxanes afforded thermally robust polysiloxazane solids, and the dehydrocoupling of 1,3,5,7-tetramethylcyclotetrasiloxane with ammonia afforded a polysiloxazane having a weight-average molecular weight of 4300 g/mol. A representative oligosilazane has been applied to a copper surface and found to afford a 20 μm thick coating that resists corrosion after 24 h under water. Addition of ammonia to [(2,6-iPr2PhBDI)Mn(µ-H)]2 allowed for characterization of the catalyst resting state, [(2,6-iPr2PhBDI)Mn(µ-NH2)]2, which has been found to mediate Si‒N dehydrocoupling.more » « less
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