Vitrimer is a new, exciting class of sustainable polymers with healing abilities due to their dynamic covalent adaptive networks. However, a limited choice of constituent molecules restricts their property space and potential applications. To overcome this challenge, an innovative approach coupling molecular dynamics (MD) simulations and a novel graph variational autoencoder (VAE) model for inverse design of vitrimer chemistries with desired glass transition temperature (T_g) is presented. The first diverse vitrimer dataset of one million chemistries is curated and T_g for 8,424 of them is calculated by high-throughput MD simulations calibrated by a Gaussian process model. The proposed VAE employs dual graph encoders and a latent dimension overlapping scheme which allows for individual representation of multi-component vitrimers. High accuracy and efficiency of the framework are demonstrated by discovering novel vitrimers with desirable T_g beyond the training regime. To validate the effectiveness of the framework in experiments, vitrimer chemistries are generated with a target T_g = 323 K. By incorporating chemical intuition, a novel vitrimer with T_g of 311–317 K is synthesized, experimentally demonstrating healability and flowability. The proposed framework offers an exciting tool for polymer chemists to design and synthesize novel, sustainable polymers for various applications.

Spider's webs are elegant examples of natural composites that can absorb out-of-plane impact energy to capture prey. Different spiders have different methods and structure of webs, and these variations in topologies have a significant effect on the prey catching abilities of the web. Taking inspiration from the spiders, metamaterials that have architectured topology can be fabricated according to end applications such as energy absorbers or impact tolerant materials. In this investigation, we theoretically examined impact loading on various orb-spider webs modeled with metamaterial architecture using materials that show size-dependent behavior. Using the size-dependent properties of nano-reinforced polymer-derived ceramics (PDCs), various metamaterial topologies were evaluated for out-of-plane impact due using ANSYS Ls-Dyna. The material properties capture the size dependency of the ceramics where smaller elements have higher strength due to reduced flaw intensity; the mechanical strength of these elements does not follow the conventional Griffith Theory. In this study, spider web geometries fabricated with PDCs with varying size elements were examined.