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CO2-induced dynamic covalent polymer networks (DCPNs) have received significant attention due to their capability of sequestering CO2 to remodel material properties. Despite the promising success of carbon sequestration in the polymer, the mechanistic understanding of the CO2-induced polymer network is still at the very beginning. A theoretical framework to understand the CO2-induced formation of bulk networks and healing of interfacial cracks of DCPNs has not been established. Here, we build up a polymer-network-based theoretical model system that can mechanistically explain the constitutive behavior and crack healing of CO2-induced DCPNs. We assume that the DCPN consists of interpenetrating networks crosslinked by CO2-induced dynamic bonds which follow a force-dependent chemical kinetics. During the healing process, we consider the CO2 molecules diffuse from the surface to the crack interface to reform the polymer network for interfacial repair. Our theoretical framework can calculate the stress-strain behaviors of both original and healed DCPNs. We demonstrate that the theoretically calculated stress-strain responses of the original DCPNs across various CO2 concentrations, as well as those of healed DCPNs under different CO2 concentrations, consistently match the documented experimental results. We expect our model to become an invaluable tool for innovating, designing, understanding, and optimizing CO2-induced DCPNs. 

Microplastic pollution constitutes a substantially detrimental type of environmental contamination and poses threats to human health. Among the sources of airborne and marine microplastics, evidence indicates that non-exhaust emissions resulting from tire abrasion and other organic materials have emerged as a notable contributor. However, the mechanistic understanding of abrasion emission of organic materials has remained elusive. To fill the gap, we here develop a multi-scale abrasion mechanics model using the principles of linear elastic fracture mechanics. Macroscopically, material wear and tear can be viewed as a process of macro-crack propagation associated with the fatigue fracture. Microscopically, we consider the effect of microcracks propagating under cyclic loading on the material modulus and energy release rate during fatigue fracture. This framework leads to an evaluation of the effective energy release rate for the abrasion-induced emission of particulate matter, thus leading to a calculation of the concentration of the emitted particulate matter with varied sizes. The theory is validated by corresponding experiments and high consistency is exhibited between the theoretical and experimental results. This research constructs a quantitative relationship between fracture mechanics and abrasion emissions. This research not only paves the way for a mechanistic understanding of particulate matter pollution from a solid mechanics perspective but also offers rational guidance for modern society to alleviate airborne particulate matter and marine microplastic abrasion emissions. 

Abstract In response to environmental stressors, biological systems exhibit extraordinary adaptive capacity by turning destructive environmental stressors into constructive factors; however, the traditional engineering materials weaken and fail. Take the response of polymers to an aquatic environment as an example: Water molecules typically compromise the mechanical properties of the polymer network in the bulk and on the interface through swelling and lubrication, respectively. Here, we report a class of 3D-printable synthetic polymers that constructively strengthen their bulk and interfacial mechanical properties in response to the aquatic environment. The mechanism relies on a water-assisted additional cross-linking reaction in the polymer matrix and on the interface. As such, the typically destructive water can constructively enhance the polymer’s bulk mechanical properties such as stiffness, tensile strength, and fracture toughness by factors of 746% to 790%, and the interfacial bonding by a factor of 1,000%. We show that the invented polymers can be used for soft robotics that self-strengthen matrix and self-heal cracks after training in water and water-healable packaging materials for flexible electronics. This work opens the door for the design of synthetic materials to imitate the constructive adaptation of biological systems in response to environmental stressors, for applications such as artificial muscles, soft robotics, and flexible electronics. 

The mechanical properties of engineering structures continuously weaken during service life because of material fatigue or degradation. By contrast, living organisms are able to strengthen their mechanical properties by regenerating parts of their structures. For example, plants strengthen their cell structures by transforming photosynthesis-produced glucose into stiff polysaccharides. In this work, we realize hybrid materials that use photosynthesis of embedded chloroplasts to remodel their microstructures. These materials can be used to three-dimensionally (3D)-print functional structures, which are endowed with matrix-strengthening and crack healing when exposed to white light. The mechanism relies on a 3D-printable polymer that allows for an additional cross-linking reaction with photosynthesis-produced glucose in the material bulk or on the interface. The remodeling behavior can be suspended by freezing chloroplasts, regulated by mechanical preloads, and reversed by environmental cues. This work opens the door for the design of hybrid synthetic-living materials, for applications such as smart composites, lightweight structures, and soft robotics. 

Abstract Emerging transformable lattice structures provide promising paradigms to reversibly switch lattice configurations, thereby enabling their properties to be tuned on demand. The existing transformation mechanisms are limited to nonfracture deformation, such as origami, instability, shape memory, and liquid crystallinity. In this study, we present a class of transformable lattice structures enabled by fracture and shape-memory-assisted healing. The lattice structures are additively manufactured with a molecularly designed photopolymer capable of both fracture healing and shape memory. We show that 3D-architected lattice structures with various volume fractions can heal fractures and fully restore stiffness and strength over two to ten healing cycles. In addition, coupled with the shape-memory effect, the lattice structures can recover fracture-associated distortion and then heal fracture interfaces, thereby enabling healing of lattice wing damages, mode-I fractures, dent-induced crashes, and foreign-object impacts. Moreover, by harnessing the coupling of fracture and shape-memory-assisted healing, we demonstrate reversible configuration transformations of lattice structures to enable switching among property states of different stiffnesses, vibration transmittances, and acoustic absorptions. These healable, memorizable, and transformable lattice structures may find broad applications in next-generation aircraft panels, automobile frames, body armor, impact mitigators, vibration dampers, and acoustic modulators.