3D printable elastomers with exceptional strength and toughness.

Three-dimensional (3D) printing has emerged as an attractive manufacturing technique because of its exceptional freedom in accessing geometrically complex customizable products. Its potential for mass manufacturing, however, is hampered by its low manufacturing efficiency (print speed) and insufficient product quality (mechanical properties). Recent progresses in ultra-fast 3D printing of photo-polymers have alleviated the issue of manufacturing efficiency, but the mechanical performance of typical printed polymers still falls far behind what is achievable with conventional processing techniques.

Regulating Hydrogen/Oxygen Species Adsorption via Built-in Electric Field -Driven Electron Transfer Behavior at the Heterointerface for Efficient Water Splitting.

Alkaline water electrolysis (AWE) plays a crucial role in the realization of a hydrogen economy. The design and development of efficient and stable bifunctional catalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are pivotal to achieving high-efficiency AWE. Herein, WC/MoC nanoparticle-embedded carbon nanofiber (WC/MoC@CNF) with abundant interfaces is successfully designed and synthesized.

Multishape Programming of Shape Memory Polymer Assemblies Fabricated by Vat Photopolymerization-Based 3D Printing and Interfacial Welding.

The combination of three-dimensional (3D) printing and shape memory polymers (SMP) enables programmable shape morphing of complex 3D structures, which is commonly termed four-dimensional (4D) printing. The process requirements of vat photopolymerization-based 3D printing impose limitations on the molecular structure design of SMPs, making it challenging to achieve triple- or multiple-shaped memory effects. Herein, we printed SMPs with different values and obtained an SMP assembly through interfacial welding.

Efficient synthesis of 6-membered cyclic monothiocarbonates from halohydrin and carbonyl sulfide.

We report herein an efficient method to synthesize 6-membered cyclic monothiocarbonates which are important intermediates for polymonothiocarbonate synthesis the cycloaddition of carbonyl sulfide with 1,3-halohydrin using a low-cost base such as triethylamine and potassium carbonate. This protocol features excellent selectivity and efficiency, mild reaction conditions and easy-to-obtain starting materials.

3D printing of dynamic covalent polymer network with on-demand geometric and mechanical reprogrammability.

Delicate geometries and suitable mechanical properties are essential for device applications of polymer materials. 3D printing offers unprecedented versatility, but the geometries and mechanical properties are typically fixed after printing. Here, we report a 3D photo-printable dynamic covalent network that can undergo two independently controllable bond exchange reactions, allowing reprogramming the geometry and mechanical properties after printing.

Regenerative Living 4D Printing via Reversible Growth of Polymer Networks.

Living creatures possess complex geometries, exceptional adaptability, and continuous growing and regenerating characteristics, which are difficult for synthetic materials to imitate simultaneously. A living polymer network with these features is reported. The polymer can be digitally printed into arbitrary 3D shapes and subsequently undergoes growth via living polymerization of a monomer as the nutrient.

Reconfigurable Polymer Networks for Digital Light Processing 3D Printing.

To realize a wide range of applications using three-dimensional (3D) printing, it is urgent to develop 3D printing resins with different functions. However, the design freedom of the resin formulation is greatly limited to guarantee fast gelation during 3D printing. Herein, we report a reconfigurable polymer network that is compatible with digital light processing (DLP) 3D printing.

Synergetic Chemical and Physical Programming for Reversible Shape Memory Effect in a Dynamic Covalent Network with Two Crystalline Phases.

A recently emerged reversible shape memory effect greatly extends the capability of shape memory polymers and their practical potential. Physical confinement and chemical fixation are individually known to be effective in introducing network anisotropy essential for reversible shape memory. Herein, we demonstrate that synergetic combination of these two mechanisms effectively diversifies the shape-shifting behavior.

Climbing-inspired twining electrodes using shape memory for peripheral nerve stimulation and recording.

Peripheral neuromodulation has been widely used throughout clinical practices and basic neuroscience research. However, the mechanical and geometrical mismatches at current electrode-nerve interfaces and complicated surgical implantation often induce irreversible neural damage, such as axonal degradation. Here, compatible with traditional 2D planar processing, we propose a 3D twining electrode by integrating stretchable mesh serpentine wires onto a flexible shape memory substrate, which has permanent shape reconfigurability (from 2D to 3D), distinct elastic modulus controllability (from ~100 MPa to ~300 kPa), and shape memory recoverability at body temperature.

Healable, Reconfigurable, Reprocessable Thermoset Shape Memory Polymer with Highly Tunable Topological Rearrangement Kinetics.

The unique capability of topological rearrangement for dynamic covalent polymer networks has enabled various unusual properties (self-healing, solid-state plasticity, and reprocessability) that are not found in conventional thermosets. Achieving these properties in one network in a synergetic fashion can open up new opportunities for shape memory polymer. To accomplish such a goal, the freedom to tune topological rearrangement kinetics is critical.

Catalyst-Free Thermoset Polyurethane with Permanent Shape Reconfigurability and Highly Tunable Triple-Shape Memory Performance.

Thermoset shape memory polymer (SMP) with dynamic covalent bonds in the network is a new class of SMPs for which the permanent shape can be reconfigured via topological rearrangement (plasticity). Catalyzed transcarbamoylation has recently been established as an effective exchange reaction for plasticity in cross-linked polyurethane networks. However, ensuring the plasticity severely constrains the network design which adversely affects the ability to tune other classical shape memory properties for practical applications.

Thermoset Shape-Memory Polyurethane with Intrinsic Plasticity Enabled by Transcarbamoylation.

Thermoset polymers are known for their superior thermomechanical properties, but the chemical crosslinking typically leads to intractability. This is reflected in the great differences between thermoset and thermoplastic shape-memory polymers; the former exhibit a robust shape memory but are not capable of redefining the permanent shape. Contrary to current knowledge, we reveal here that a classical thermoset shape-memory polyurethane is readily capable of permanent reshaping (plasticity) after a topological network rearrangement that is induced by transcarbamoylation.