The plating/stripping of Li dendrites can fracture the static solid electrolyte interphase (SEI) and cause significant dynamic volume variations in the Li anode, which give rise to poor cyclability ...and severe safety hazards. Herein, a tough polymer with a slide‐ring structure was designed as a self‐adaptive interfacial layer for Li anodes. The slide‐ring polymer with a dynamically crosslinked network moves freely while maintaining its toughness and fracture resistance, which allows it can to dissipate the tension induced by Li dendrites on the interphase layer. Moreover, the slide‐ring polymer is highly stretchable, elastic, and displays an ultrafast self‐healing ability, which allows even pulverized Li to remain coalesced without disintegrating upon consecutive cycling. The Li anodes demonstrate greatly improved suppression of Li dendrite formation, as evidenced by the high critical current density (6 mA cm−2) and stable cycling for the full cells with high‐areal capacity LiFePO4, high‐voltage NCM, and S cathodes.
A slide‐ring polymer with a high stiffness, high toughness and excellent fracture resistance is designed to adapt its shape to dynamic electrode volume variations and stabilize the lithium anode upon cycling.
The uncontrolled growth of Li dendrites upon cycling might result in low coulombic efficiency and severe safety hazards. Herein, a lithiophilic binary lithium–aluminum alloy layer, which was ...generated through an in situ electrochemical process, was utilized to guide the uniform metallic Li nucleation and growth, free from the formation of dendrites. Moreover, the formed LiAl alloy layer can function as a Li reservoir to compensate the irreversible Li loss, enabling long‐term stability. The protected Li electrode shows superior cycling over 1700 h in a Li|Li symmetric cell.
Dendrite‐free anodes: An efficient lithium–aluminum alloy medium with increased affinity for Li and generated through an in situ electrochemical process is engineered to guide uniform Li nucleation and suppress the growth of Li dendrites.
A mechanically robust, ultraelastic foam with controlled multiscale architectures and tunable mechanical/conductive performance is fabricated via 3D printing. Hierarchical porosity, including both ...macro‐ and microscaled pores, are produced by the combination of direct ink writing (DIW), acid etching, and phase inversion. The thixotropic inks in DIW are formulated by a simple one‐pot process to disperse duo nanoparticles (nanoclay and silica nanoparticles) in a polyurethane suspension. The resulting lightweight foam exhibits tailorable mechanical strength, unprecedented elasticity (standing over 1000 compression cycles), and remarkable robustness (rapidly and fully recover after a load more than 20 000 times of its own weight). Surface coating of carbon nanotubes yields a conductive elastic foam that can be used as piezoresistivity sensor with high sensitivity. For the first time, this strategy achieves 3D printing of elastic foam with controlled multilevel 3D structures and mechanical/conductive properties. Moreover, the facile ink preparation method can be utilized to fabricate foams of various materials with desirable performance via 3D printing.
Mechanically robust hierarchical foam with unprecedented elasticity, controllable structure, and performance is fabricated by 3D printing using concentrated nanofiller‐based inks. Combination of direct ink writing, acid etching, and phase inversion produces pores in three different length scale, which are tunable through ink formulation or computer‐designed geometries. Surface coating of carbon nanotubes yields a highly sensitive stress sensor with excellent recoverability.
The growth of white‐rot fungi is related to the superior infiltrability and biodegradability of hyphae on a lignocellulosic substrate. The superior biodegradability of fungi toward plant substrates ...affords tailored microstructures, which benefits subsequently high efficient carbonization and chemical activation. Here, the mechanism underlying the direct growth of mushrooms toward the lignocellulosic substrate is elucidated and a fungi‐enabled method for the preparation of porous carbons with ultrahigh specific surface area (3439 m2 g−1) is developed. Such porous carbons could have potential applications in energy storage, environment treatment, and electrocatalysis. The present study reveals a novel pore formation mechanism in root‐colonizing fungi and anticipates a valuable function for fungi in developing the useful porous carbons with a high specific surface area.
A universal fungi‐enabled method for the preparation of porous carbons with ultrahigh specific surface area for energy storage, adsorption, and electrocatalysis is developed. Hyphae infiltrate into the plant cell wall to secrete corresponding exoenzymes to generate a multidimensional framework, which is beneficial to the following carbonization and activation process.
Realizing solid‐state lithium batteries with higher energy density and enhanced safety compared to the conventional liquid lithium‐ion batteries is one of the primary research and development goals ...set for next‐generation batteries in this decade. In this regard, polymer electrolytes have been widely researched as solid electrolytes due to their excellent processability, flexibility, and low weight. With high cationic transference numbers (tLi+ close to 1), single‐ion conducting polymer electrolytes (SICPEs) have tremendous advantages compared to polymer electrolyte systems (tLi+ < 0.4) because of their potential to reduce the buildup of ion concentration gradients and suppress growth of lithium dendrites. The current review covers the fundamentals of SICPEs, including anionic unit synthesis, polymer structure design, and film fabrication, along with simulation and experimental results in solid‐state lithium–metal battery applications. A perspective on current challenges, possible solutions, and potential research directions of SICPEs is also discussed to provide the research community with the critical technical aspects that may advance SICPEs as solid electrolytes in next‐generation energy storage systems.
This review covers the fundamentals of single‐ion conducting polymer electrolytes (SICPEs), including anionic unit synthesis, structure design, and film fabrication, along with simulation and experimental results in solid‐state lithium‐metal batteries. A perspective on current challenges, possible solutions, and research directions of SICPEs is also discussed to provide critical aspects that may advance SICPEs as solid electrolytes in lithium‐metal batteries.
It is a great challenge to fabricate electrode with simultaneous high activity for the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER). Herein, a high‐performance ...bifunctional electrode formed by vertically depositing a porous nanoplate array on the surface of nickel foam is provided, where the nanoplate is made up by the interconnection of trinary Ni–Fe–Mo suboxides and Ni nanoparticles. The amorphous Ni–Fe–Mo suboxide and its in situ transformed amorphous Ni–Fe–Mo (oxy)hydroxide acts as the main active species for HER and OER, respectively. The conductive network built by Ni nanoparticles provides rapid electron transfer to active sites. Moreover, the hydrophilic and aerophobic electrode surface together with the hierarchical pore structure facilitate mass transfer. The corresponding water electrolyzer demonstrates low cell voltage (1.50 V @ 10 mA cm−2 and 1.63 V @ 100 mA cm−2) with high durability at 500 mA cm−2 for at least 100 h in 1 m KOH.
A high‐performance bifunctional electrode in the form of a porous nanoplate array vertically aligned on nickel foam for overall water splitting is provided. The porous nanoplate is built by the interconnection of trinary Ni–Fe–Mo suboxides and Ni nanoparticles, which is featured with amorphous active material and rapid electron/mass transfer.
Highly elastic silicone foams, especially those with tunable properties and multifunctionality, are of great interest in numerous fields. However, the liquid nature of silicone precursors and the ...complicated foaming process hinder the realization of its three‐dimensional (3D) printability. Herein, a series of silicone foams with outstanding performance with regards to elasticity, wetting and sensing properties, multifunctionality, and tunability is generated by direct ink writing. Viscoelastic inks are achieved from direct dispersion of sodium chloride in a unique silicone precursor solution. The 3D‐architectured silicone rubber exhibits open‐celled trimodal porosity, which offers ultraelasticity with hyper compressibility/cycling endurance (near‐zero stress/strain loss under 90% compression or 1000 compression cycles), excellent stretchability (210% strain), and superhydrophobicity. The resulting foam is demonstrated to be multifunctional, such that it can work as an oil sorbent with super capacity (1320%) and customizable soft sensor after absorption of carbon nanotubes on the foam surface. The strategy enables tunability of mechanical strength, elasticity, stretchability, and absorbing capacity, while printing different materials together offers property gradients as an extra dimension of tunability. The first 3D printed silicone foam, which serves an important step toward its application expansion, is achieved.
Multi‐functional, hyper‐elastic silicone foam is three‐dimensionally (3D) printed from a viscoelastic ink. Trimodal porosity is achieved to offer extreme compressibility/cyclic endurance and remarkable stretchability. The resulting foam is multi‐functional, serving as a super oil‐sorbent and soft sensor after surface‐absorption of carbon nanotubes. Tuning ink composition, designing 3D architecture, and printing different materials together afford multi‐dimensional control over foam performance.
Self‐healable elastomers are extremely attractive due to their ability to prolong product lifetime. An additional function that could further expand their applications is strong adhesion force to ...clean and dusty surfaces. This study reports a series of autonomous self‐healable and highly adhesive elastomers (ASHA‐Elastomer) that are fabricated via a simple, efficient, and scalable process. The obtained elastomers exhibit outstanding mechanical properties with elongation at break up to 2102% and toughness (modulus of toughness) of 1.73 MJ m–3. The damaged ASHA‐Elastomer can autonomously self‐heal with full recovery of functionalities, and the healing process is not affected by the presence of water. The elastomers are found to possess an ultrahigh adhesion force up to 3488 N m−1, greatly outperforming previously reported self‐healing adhesive elastomers. Furthermore, the adhesion force of the ASHA‐Elastomer is negligibly affected by dust on the surface, in stark contrast with regular adhesive polymers that have adhesion strengths extremely sensitive to dust. The successful development of high‐toughness, autonomous self‐healable, and ultra‐adhesive elastomers will enable a wide range of applications with enhanced longevity and versatility, including their use in sealants, adhesives, and stretchable devices.
A series of self‐healing adhesive elastomers are fabricated via a simple, efficient, and scalable process. The obtained elastomers exhibit outstanding mechanical properties (extensibility 2102%, toughness 1.73 MJ m–3), and the damaged areas can autonomously self‐heal with full recovery. They also possess an ultrahigh adhesion force (3488 N m−1), greatly exceeding the reported self‐healing adhesive elastomers.
An optimized nanostructure design for high‐power, high‐energy lithium‐ion batteries and supercapacitors is realized by fabricating a nanocomposite with highly dispersed nanoparticles of active ...materials in a nanoporous carbon matrix. A nano‐LiFePO4/nanoporous carbon matrix nanocomposite forms a bridge between a supercapacitor and a battery electrode and offers a reasonable compromise between rate and capacity.
Layered Ni‐rich lithium transition metal oxides are promising battery cathodes due to their high specific capacity, but their poor cycling stability due to intergranular cracks in secondary particles ...restricts their practical applications. Surface engineering is an effective strategy for improving a cathode's cycling stability, but most reported surface coatings cannot adapt to the dynamic volume changes of cathodes. Herein, a self‐adaptive polymer (polyrotaxane‐co‐poly(acrylic acid)) interfacial layer is built on LiNi0.6Co0.2Mn0.2O2. The polymer layer with a slide‐ring structure exhibits high toughness and can withstand the stress caused by particle volume changes, which can prevent the cracking of particles. In addition, the slide‐ring polymer acts as a physicochemical barrier that suppresses surface side reactions and alleviates the dissolution of transition metallic ions, which ensures stable cycling performance. Thus, the as‐prepared cathode shows significantly improved long‐term cycling stability in situations in which cracks may easily occur, especially under high‐rate, high‐voltage, and high‐temperature conditions.
A slide‐ring polymer featuring high elasticity and self‐adaptive ability is designed to improve the performance of lithium‐ion batteries via relieving the cracks of cathode particles and retarding parasitic interfacial side reactions during cycling.
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