Interface compatible organic-inorganic solid electrolyte with intimate electrode/electrolyte interfacial contact for dendrite-free Li metal batteries.

The increasing demand for safe, high-energy-density batteries drives the development of solid-state electrolytes. Organic/inorganic hybrid electrolytes, integrating the benefits of polymer and inorganic electrolytes, exhibit flexibility, high mechanical strength, and superior ionic conductivity. However, interfacial incompatibility between organic/inorganic components and high electrolyte/electrode interfacial resistance restricts their practical applications.

Polyimide-driven innovations as "inert" components in high-performance lithium-ion batteries.

The rapid proliferation of lithium-ion batteries (LIBs) across portable electronics and electrified transportation systems has propelled unprecedented requirements for high energy density, prolonged cycle life, and improved safety protocols. Polyimides (PIs), attributed to the excellent thermal stability, mechanical robustness, chemical stability, and flame retardant properties, have been widely researched as "inert" materials to address critical challenges in advancing LIBs. Herein, this review provides design principles for employing PIs' inherent characteristics to develop next-generation high-performance LIBs with balanced energy density, rate capability, and operational reliability.

Closed-Loop and Selective Recyclable Fluoro-Containing Graft Copolymers with Diverse Applications.

The intrinsic chemically inert fluoropolymers, constitute a large portion of per- and polyfluoroalkyl substances (PFAS), granting them unique properties and prolonged lifetime while also bring substantial environmental concerns. This study develops fluoro-containing graft copolymer with closed-loop and selective recyclability of side chains. The poly(vinylidene fluoride-co-chlorotrifluoroethylene) (PVDF-CTFE) backbone is modified via 4-vinylbenzyl alcohol (VBOH) units and then grafted by poly (trimethylene carbonate) (PTMC) side chains, yielding the graft copolymer with improved ionic conductivity and enhanced mechanical robustness, demonstrating it as a polymer electrolyte for battery application.

Catalytic remodeling of complex alkenes to oxonitriles through C=C double bond deconstruction.

Deconstructive transformation of carbon-carbon double bonds (C=C) is a pivotal strategy in synthetic chemistry and drug discovery. Despite the substantial advances in olefin metathesis and ozonolysis for natural product synthesis through C=C double-bond cleavage, the catalytic remodeling of complex molecules through C=C double-bond deconstruction has been underdeveloped. We report a heterogeneous copper-catalyzed C=C double-bond cleavage, which enables the remodeling of complex molecules by converting the carbons on either side of the C=C double bond to carbonyl and cyano groups, respectively.

Mastering the Copolymerization Behavior of Ethyl Cyanoacrylate as Gel Polymer Electrolyte for Lithium-metal Battery Application.

Polymers with strong electron-withdrawing groups (e.g., cyano-containing polymers) are attractive for a wide range of applications due to their high dielectric constant and outstanding electrochemical stability.

Ultra-robust Single-Ion Conducting Composite Electrolytes for Stable Li-Metal Batteries.

With significantly high lithium-ion (Li) transport efficiency, single-ion conducting polymer electrolytes (SIPEs) often suffer from low ionic conductivity due to the covalently bonded anions to the polymer backbone. Adding plasticizers to SIPEs to improve ionic conductivity usually reduces the polymer matrix's mechanical robustness, negatively affecting overall performance as solid electrolytes. Herein, to surpass such a trade-off relationship, we successfully designed a single-ion conducting composite membrane (c-SIPM60) with cross-linked linear SIPEs and incorporated glass-mesh substrate, which shows a cation transport number close to 1, ultrahigh tensile strength of 22 MPa (modulus of 547.

Construction of an ultrathin multi-functional polymer electrolyte for safe and stable all-solid-state batteries.

The ever-increasing demand for safe and high-energy-density batteries urges the exploration of ultrathin, lightweight solid electrolytes with high ionic conductivity. Solid polymer electrolytes (SPEs) with high flexibility, reduced interfacial resistance and excellent processability have been attracting significant attentions. However, reducing the thickness of SPEs to be comparable with that of commercial separators increases the risk of short-circuiting.

Covalent adaptable polymer networks with CO-facilitated recyclability.

Cross-linked polymers with covalent adaptable networks (CANs) can be reprocessed under external stimuli owing to the exchangeability of dynamic covalent bonds. Optimization of reprocessing conditions is critical since increasing the reprocessing temperature costs more energy and even deteriorates the materials, while reducing the reprocessing temperature via molecular design usually narrows the service temperature range. Exploiting CO gas as an external trigger for lowering the reprocessing barrier shows great promise in low sample contamination and environmental friendliness.

Design of PDMS/PAN composite membranes with ultra-interfacial stability layer integration.

The interfacial interaction between the selective layer and porous substrate directly determines the separation performance and service lifetime of functional composite membranes. Till now, almost all reported polymeric selective layers are physically in contact with the substrate, which is unsatisfactory for long-term operation. Herein, we introduced a functional composite membrane with ultra-interfacial stability layer integration between the polydimethylsiloxane selective layer and polyacrylonitrile substrate, where a facile light-triggered copolymerization achieved their covalent bonding.

Tuning the Mechanical and Dynamic Properties of Elastic Vitrimers by Tailoring the Substituents of Boronic Ester.

Elastic vitrimers, i.e., elastic polymers with associative dynamic covalent bonds, can afford elastomers with recyclability while maintaining their thermal and chemical stability.

Hybrid Dynamic Covalent Network-Based Protecting Layer for Stable Li-Metal Batteries.

Metallic lithium (Li) is considered as the "Holy Grail" anode material for next-generation energy storage systems due to its extremely high theoretical capacity and low electrochemical potential. Before the commercialization of the Li electrode, dendritic Li growth and the unstable solid electrolyte interphase layer should be conquered. Herein, a hybrid covalent adaptable polymer network (HCAPN) is prepared via the random copolymerization of poly(ethylene glycol) methyl ether methacrylate and -acetoacetoxyethyl methacrylate, followed by chemical cross-linking with polyethylenimine (PEI) and amine-modified silicon dioxide (SiO).

Superstretchable Liquid-Metal Electrodes for Dielectric Elastomer Transducers and Flexible Circuits.

Dielectric elastomer transducers (DETs), with a dielectric elastomer (DE) film sandwiched between two compliant electrodes, are highly sought after in the fields of soft robotics, energy harvesting, and human-machine interaction. To achieve a high-performance DET, it is essential to develop electrodes with high conductivity, strain-insensitive resistance, and adaptability. Herein, we design an electrode (Supra-LMNs) based on multiple dynamic bond cross-linked supramolecular networks (Ns) and liquid metal (LM), which realizes high conductivity (up to 16,000 S cm), negligible resistance changes at high strain (1.

Ductile adhesive elastomers with force-triggered ultra-high adhesion strength.

Elastomers play a vital role in many forthcoming advanced technologies in which their adhesive properties determine materials' interface performance. Despite great success in improving the adhesive properties of elastomers, permanent adhesives tend to stick to the surfaces prematurely or result in poor contact depending on the installation method. Thus, elastomers with on-demand adhesion that is not limited to being triggered by UV light or heat, which may not be practical for scenarios that do not allow an additional external source, provide a solution to various challenges in conventional adhesive elastomers.

Selective deconstruction of mixed plastics by a tailored organocatalyst.

Plastic represents an essential material in our society; however, a major imbalance between their high production and end-of-life management is leading to unrecovered energy, economic hardship, and a high carbon footprint. The adoption of plastic recycling has been limited, mainly due to the difficulty of recycling mixed plastics. Here, we report a versatile organocatalyst for selective glycolysis of diverse consumer plastics and their mixed waste streams into valuable chemicals.

Puncture-resistant self-healing polymers with multi-cycle adhesion and rapid healability.

The structural design of self-healing materials determines the ultimate performance of the product that can be used in a wide range of applications. Incorporating intrinsic self-healing moieties into puncture-resistant materials could significantly improve the failure resistance and product longevity, since their rapidly rebuilt bonds will provide additional recovery force to resist the external force. Herein, we present a series of tailored urea-modified poly(dimethylsiloxane)-based self-healing polymers (U-PDMS-SPs) that exhibit excellent puncture-resistant properties, fast autonomous self-healing, multi-cycle adhesion capabilities, and well-tunable mechanical properties.

Hybrid Dynamic Covalent Network as a Protective Layer and Solid-State Electrolyte for Stable Lithium-Metal Batteries.

Lithium (Li) metal is a highly promising anode material for next-generation high-energy-density batteries, while Li dendrite growth and the unstable solid electrolyte interphase layer inhibit its commercialization. Herein, a chemically grafted hybrid dynamic network (CHDN) is rationally designed and synthesized by the 4,4'-thiobisbenzenamine cross-linked poly(poly(ethylene glycol) methyl ether methacrylate--glycidyl methacrylate) and (3-glycidyloxypropyl) trimethoxysilane-functionalized SiO nanoparticles, which is utilized as a protective layer and hybrid solid-state electrolyte (HSE) for stable Li-metal batteries. The presence of a dynamic exchangeable disulfide affords self-heability and recyclability, and the chemical attachment between SiO nanoparticles and the polymer matrix enables the homogeneous distribution of inorganic fillers and mechanical robustness.

Intrinsically Self-Healing Polymers: From Mechanistic Insight to Current Challenges.

Self-healing materials open new prospects for more sustainable technologies with improved material performance and devices' longevity. We present an overview of the recent developments in the field of intrinsically self-healing polymers, the broad class of materials based mostly on polymers with dynamic covalent and noncovalent bonds. We describe the current models of self-healing mechanisms and discuss several examples of systems with different types of dynamic bonds, from various hydrogen bonds to dynamic covalent bonds.

Single-Ion Conducting Polymeric Protective Interlayer for Stable Solid Lithium-Metal Batteries.

With many reported attempts on fabricating single-ion conducting polymer electrolytes, they still suffer from low ionic conductivity, narrow voltage window, and high cost. Herein, we report an unprecedented approach on improving the cationic transport number () of the polymer electrolyte, , single-ion conducting polymeric protective interlayer (SIPPI), which is designed between the conventional polymer electrolyte (PVEC) and Li-metal electrode. Satisfied ionic conductivity (1 mS cm, 30 °C), high (0.

Unravelling the Influence of Surface Modification on the Ultimate Performance of Carbon Fiber/Epoxy Composites.

The overall performance of polymer composites depends on not only the intrinsic properties of the polymer matrix and inorganic filler but also the quality of interfacial adhesion. Although many reported approaches have been focused on the chemical treatment for improving interfacial adhesion, the examination of ultimate mechanical performance and long-term properties of polymer composites has been rarely investigated. Herein, we report carbon fiber (CF)/epoxy composites with improved interfacial adhesion by covalent bonding between CFs and the epoxy matrix.

On the Interfacial Behavior of Catenated Poly(l-lactide) at the Air-Water Interface.

Interfacial properties of polymeric materials are significantly influenced by their architectural structures and spatial features, while such a study of topologically interesting macromolecules is rarely reported. In this work, we reported, for the first time, the interfacial behavior of catenated poly(l-lactide) (C-PLA) at the air-water interface and compared it with its linear analogue (L-PLA). The isotherms of surface pressure-area per repeating unit showed significant interfacial behavioral differences between the two polymers with different topologies.

Self-Healable, Highly Stretchable, Ionic Conducting Polymers as Efficient Protecting Layers for Stable Lithium-Metal Electrodes.

Although numerous studies on polymeric protective films to stabilize lithium (Li)-metal electrodes have been reported, the construction of self-healing polymers that enables the long-term operation of Li-metal batteries (LMBs) at relatively low temperatures has rarely been demonstrated. Herein, a highly stretchable, autonomous self-healable, and ionic-conducting polymer network (SHIPN) is synthesized as an efficient protective film for LMBs. The network backbone, synthesized from copolymerization of poly(ethylene glycol)-mono-methacrylate (PEGMMA) and 2-[[(butylamino)carbonyl]oxy]ethyl acrylate (BCOE), is chemically cross-linked via diisocyanate.

Unravelling the Mechanism of Viscoelasticity in Polymers with Phase-Separated Dynamic Bonds.

Incorporation of dynamic (reversible) bonds within polymer structure enables properties such as self-healing, shape transformation, and recyclability. These dynamic bonds, sometimes refer as stickers, can form clusters by phase-segregation from the polymer matrix. These systems can exhibit interesting viscoelastic properties with an unusually high and extremely long rubbery plateau.

Turning Rubber into a Glass: Mechanical Reinforcement by Microphase Separation.

Supramolecular associations provide a promising route to functional materials with properties such as self-healing, easy recyclability or extraordinary mechanical strength and toughness. The latter benefit especially from the transient character of the formed network, which enables dissipation of energy as well as regeneration of the internal structures. However, recent investigations revealed intrinsic limitations in the achievable mechanical enhancement.