Interfacial Compatibility Research Articles

Prolonging rechargeable aluminum batteries life with flexible ceramic separator

Rechargeable aluminum batteries (RABs) are attracting significant attention for their high theoretical capacity and abundant reserves. However, the poor mechanical performance of glass fiber (GF) separators and the formation of Al dendrite severely hinder the practical cycle life of these batteries. Herein, a flexible ceramic separator was developed with simple coating technique, effectively improving the cycling stability of RABs. Compared with the commercial GF separator, this flexible ceramic separator has less thickness and superior electrolyte wettability, resulting in improved interfacial compatibility and minimized interfacial resistance. Moreover, its exceptional flexibility and toughness (stress of 39.34 MPa) coupled with uniform nanopore structure, which can effectively resist the penetration of dendrites. As expected, this ceramic flexible separator facilitates stable cycling of the symmetric battery for over 1762 h at 2 mA/cm2 and 2 mAh/cm2. It also permits the pouch Al//flake graphite full battery to achieve a coulombic efficiency of up to 90% even after 115 cycles. Apparently, this work developed the simple separator manufacturing strategy that provides an effective method to improve the cycling stability of RABs and extends the application to other types of batteries.

Innovative bamboo-plastic composites interfacial compatibility design approach: Self-assembled crosslinked structure of polydopamine with acylated chitin fibers

Achieving interfacial compatibility through sustainable methods is a key objective in natural fiber-plastic composites research, aimed at optimizing mechanical performance. This study introduced an innovative organic bamboo-plastic composite (BPC) interfacial layer, incorporating O-acylated chitin fibers densely coated with polydopamine (PDA) via a mild and facile self-assembly method. Chitin nanofibers were acylated with dodecenylsuccinic anhydride in a deep eutectic solvent in a one-pot process. The resulting BPCs exhibited significantly enhanced mechanical properties, with tensile strength, flexural strength, modulus, and impact strength increased by 73.64 %, 39.19 %, 15.42 %, and 63.57 %, respectively, compared to untreated BPCs. This improvement highlights the effectiveness of tailoring cross-linked networks across heterogeneous interfaces in providing strength, dissipating strain, and promoting interfacial compatibility. Furthermore, these modified BPCs demonstrated enhanced thermal stability, crystallization behavior, and moderate hydrophobicity. This surface treatment strategy offers a distinctive approach to producing high-performance, eco-friendly BPCs, also facilitating the processing and utilization of marine biological resources on a wide scale.

A Comprehensive Review of Functional Gel Polymer Electrolytes and Applications in Lithium-Ion Battery.

The rapid expansion of flexible and wearable electronics has necessitated a focus on ensuring their safety and operational reliability. Gel polymer electrolytes (GPEs) have become preferred alternatives to traditional liquid electrolytes, offering enhanced safety features and adaptability to the design requirements of flexible lithium-ion batteries. This review provides a comprehensive and critical overview of recent advancements in GPE technology, highlighting significant improvements in its physicochemical properties, which contribute to superior long-term cycling stability and high-rate capacity compared with traditional organic liquid electrolytes. Special attention is given to the development of smart GPEs endowed with advanced functionalities such as self-protection, thermotolerance, and self-healing properties, which further enhance battery safety and reliability. This review also critically examines the application of GPEs in high-energy cathode materials, including lithium nickel cobalt manganese (NCM), lithium nickel cobalt aluminum (NCA), and thermally stable lithium iron phosphate (LiFePO4). Despite the advancements, several challenges in GPE development remain unresolved, such as improving ionic conductivity at low temperatures and ensuring mechanical integrity and interfacial compatibility. This review concludes by outlining future research directions and the remaining technical hurdles, providing valuable insights to guide ongoing and future efforts in the field of GPEs for lithium-ion batteries, with a particular emphasis on applications in high-energy and thermally stable cathodes.

Nano-sulfur decorated graphene oxide to improve the mechanical properties of natural rubber by interfacial participate in the vulcanization reaction

As a new material with excellent comprehensive properties, graphene is an excellent reinforcing agent for natural rubber (NR). However, how to improve the interface performance between graphene and NR, and at the same time be practical, is still a great challenge. In this study, nano-sulfur decorated graphene oxide materials (GO-S) were prepared by in-situ loading nano-sulfur on the surface of graphene oxide (GO). Nano-surface cross-link with NR in the vulcanization process, acts as a bridge to anchor GO and NR molecular chains and improve the interface bonding strength of GO and NR. The AFM results show that the interfacial phase thickness of NR-GO-S composites increased from 135 ± 18 nm to 245 ± 28 nm after in-situ loading modification. The tensile strength and tear property of NR-GO-S composites modified by sulfur loading reach 30.3 MPa and 40.0 kN⋅m−1, respectively, which are 31.1 % and 12.8 % higher than those of NR-GO composite. Nano-sulfur form O–S and C–S covalent bonds with GO, and form more efficient covalent crosslinking networks with NR molecules in the vulcanization process, thus improving the interfacial compatibility between GO and NR and making the load transfer in rubber matrix more effective. This work provides a new idea and method to improve the interface property between rubber and inorganic nanomaterials.

Porous organic cage induced high CO2/CH4 separation efficiency of carbon molecular sieve membranes

Porous fillers have been incorporated into precursor membranes to fabricate carbon molecular sieve (CMS) membranes, where the interfacial compatibility between fillers and matrix significantly influences the separation performance of converted CMS membranes. To address this issue, we introduce molecular fillers of porous organic cages (POCs) into precursor membranes, the organic composition and discrete molecular characteristics of which can enhance the compatibility with the polymer matrix (PIM-1), bringing enhanced porosity and narrowed pore size distribution, especially in the ultra-micropore region, to the CMS membranes. The obtained CMS membrane shows simultaneously improved gas permeability and selectivity wherein the optimized CMS membrane pyrolyzed at 600 °C with 10 wt% POCs loading (CMS-10%-600) exhibits a CO2 permeability of 2002 Barrer and a CO2/CH4 selectivity of 221.6, surpassing the 2019 CO2/CH4 upper bound and superior to most of reported CMS membranes. Due to the incorporation of POC, the CMS-10%-600 membrane demonstrates a 147.5 % increase in CO2 permeability and a 297.1 % increase in CO2/CH4 selectivity compared to pristine PIM-1-based CMS membrane, along with the excellent aging resistance for over 30 days. This study provides new insights into the design of high-performance CMS membranes for gas separation.

Surface to bulk design empowering Ni-rich layered oxide cathode in sulfide-based All-Solid-State batteries

All-solid-state batteries (ASSBs) employing sulfide solid electrolytes (SSE) and high-nickel layered oxide cathodes have attracted considerable attention, attributed to their superior safety and great potential for high energy densities. However, the interface compatibility between SSE and nickel-rich oxide cathode remains a challenge. Here, a dual-functional strategy of Li6.25La3Zr2Al0.25O12 surface coating and bulk Zr doping in LiNi0.8Co0.1Mn0.1O2 was proposed (NCM811@CD-LLZAO), aiming to enhance the interfacial compatibility toward sulfide-based ASSBs. The fabricated ASSBs exhibit an impressive capacity retention rate of 91.1% after 100cycles at 0.1C and can sustain an ultra-long cycling performance over 1000cycles at 1.0C. Remarkably, even at a high rate of 11.0C, the battery still maintains a high capacity, highlighting its excellent rate performance. The distribution of relaxation time (DRT) analysis reveals that the LLZAO buffering layer can enhance the kinetics at the cathode/electrolyte interface. Theoretical calculation further confirms that the strong Zr-O bond formed by Zr doping can stabilize the lattice oxygen and effectively prevent the sulfide solid electrolyte from further electrochemical oxidation, thereby enhancing the interfacial dynamic and stability. These encouraging results provide a new strategy for the practical application of high-energy–density ASSBs, enabling fast charge transfer, extended cycle longevity and enhanced safety.

A new application of MoS2@AG@PA prepared by irradiation: Synergizing with magnesium hydroxide to enhance fire safety and other key properties of EVA composites

AbstractTwo‐dimensional molybdenum disulfide (MoS2) nanosheets are seen as highly promising nanofillers for enhancing polymer properties, yet there is a need for methods that are low‐cost, simple, and environmentally friendly to facilitate the large‐scale production of MoS2 nanosheets. Furthermore, it is necessary to functionalize the MoS2 surface to ensure good interfacial compatibility with the polymer matrix. In this study, MoS2@Ag@PA hybrids were created by generating silver nanoparticles directly on the surface of MoS2 via radiation, followed by encapsulation on the surface of MoS2@Ag through the chelating properties of phytic acid. It is significant to note that, due to the excellent lubrication and physical cross‐linking effects of the MoS2@Ag@PA hybrids, adding one part of MoS2@Ag@PA hybrids can enhance the melt flow rate and elongation at break of the ethylene vinyl acetate copolymer (EVA)/MH composites by 140% and 17.3%, respectively. The simultaneous addition of one part of MoS2@Ag@PA hybrids decreased the peak heat release rate, total heat release, and total smoke release of the EVA composites by 48.7%, 42.7%, and 41.2%, respectively. Moreover, the toxic gasses (e.g., CO) generated by burning EVA composites were significantly reduced compared to pure EVA, indicating improved fire safety. This research not only provides significant opportunities for the green mass production of MoS2 nanosheets but also expands their potential applications in high‐performance nanocomposites.

An in situ gel electrolyte for the facile preparation of high‐safety Li‐S battery

AbstractLithium‐sulfur (Li‐S) battery shows promising development potential in secondary lithium‐ion batteries. However, the shuttle effect of polysulfides, uncontrollable lithium dendrite growth, and safety hazards in conventional liquid electrolytes limit the popularity of Li‐S batteries in the future commercial market. In this work, a high‐performance gel electrolyte (GPE) was prepared in situ by initiating the ring‐opening polymerization of 1,3‐dioxolane (DOL) with aluminum trifluoromethanesulfonate (Al(OTf)3) and using diethylene glycol dimethyl ether (DME) as a plasticizer, which can effectively improve the interfacial compatibility between sulfur cathode and the electrolyte, as well as the stability of lithium anode. The electrochemical performance of the poly‐DOL (PDOL) GPE was optimized by adjusting the concentration ratio of the initiator. When the concentration of Al(OTf)3 is 4 mM, the PDOL GPE has a high ionic conductivity up to 3.81 × 10−4 S cm−1 and a lithium ion migration number of 0.57. The assembled quasi‐solid‐state Li‐S batteries shows an initial discharge specific capacity of 908.1 mAh g−1 at 0.1 C with a capacity retention of 68% after 240 cycles, and its average Coulombic efficiency is maintained at 96.1%. This gel electrolyte design provides a feasible practical idea in quasi‐solid‐state Li‐S batteries.

The Effect of Zn2(BDC)2 Metal Organic Framework on the Miscibility and Properties of Poly(Lactic Acid)/Poly(Butylene Adipate-co-Terephthalate) Biodegradable Blends

In our research described in this paper, the metal-organic framework MOF-2 [Zn2(BDC)2] was used to enhance the properties of a biodegradable blend based on poly(lactic acid) (PLA) and poly(butylene adipate-co-terephthalate) (PBAT). PLA/PBAT/(1, 3, 5, and 7 wt%) MOF-2 blends were prepared using a melt blending technology with a twin-screw extruder. The phase morphology, rheological behavior and barrier properties of the blends were studied. X-ray diffraction (XRD) showed a slight increase in the crystalline content of the PLA/PBAT matrix with increasing MOF-2 content. Scanning electron microscopy (SEM) revealed that the PLA/PBAT blend was immiscible, and the phase morphology improved with MOF-2 by enhancing the interfacial compatibility, reducing the size of micro-domains and cavities, and promoting a transition to a co-continuous morphology, indicating better miscibility. The ternary nanocomposites with 5 and 7 wt% MOF-2 showed increased complex viscosity (η*) and storage modulus (G′) compared to those with 1 and 3% MOF-2, indicating stronger percolated networks. The thermal and barrier properties and water absorption capacity were also improved, confirming the rheological measurements. All the results showed that the PLA/PBAT/MOF-2 nanocomposites could be used in the field of packaging.

Characterization and Properties of Polylactic Acid/Cottonseed Protein Bioplastics

AbstractIn this study, polylactic acid (PLA) is compounded with cottonseed protein concentrate (CPC) by melt blending under the compatibilization of maleic anhydride (MA), and then hot‐pressed to prepare PLA/CPC composite bioplastics. The attenuated total reflection Fourier transform infrared (ATR‐FTIR) spectroscopy showed that high temperature and compatibilizer induced the protein secondary structure to transition. CPC can be used as a heterogeneous PLA nucleating agent, effectively accelerating PLA crystallization, which is characterized by polarization optical microscopy (POM), synchrotron radiation wide‐angle X‐ray scattering (WAXS) and differential scanning calorimetry (DSC). The highest crystallinity of the PLA/CPC10 composite is 8.9% higher than that of neat PLA. The unfolding of the protein secondary structure is likely to promote an orderly arrangement of PLA crystals, showing strong binding forces between them. Moreover, the CPC/PLA interfacial compatibility is improved by the addition of a small amount of maleic anhydride. The increased crystallinity and interfacial compatibility contribute to the improved mechanical properties, water resistance, and thermal stability of the bioplastics. Environmentally friendly plastic handicrafts (e.g., commemorative emblems, flower pots, ornaments, etc.) can be fabricated using these biocomposites for future value‐added applications.

Garnet and Li29Zr9Nb3O40 Modified PEO‐Based Hybrid Solid Electrolytes for All‐Solid‐State Lithium Metal Batteries

AbstractInorganic‐organic hybrid solid electrolytes (HSEs) are an important category of electrolyte materials for solid‐state batterie. It is of interest and importance to investigate the influence of composition and content of inorganic fillers on the electrochemical performance of HSEs. In this paper, we fabricated HSEs using polyethylene oxide (PEO) as matrix and incorporating different inorganic powders as active fillers. A series of HSEs with different contents of Ga/Nb co‐substituted garnet oxide (Li6.35Ga0.15La3Zr1.8Nb0.2O12, GN‐LLZO) and Y‐doped Li29Zr9Nb3O40 (Li29.3Zr8.7Y0.3Nb3O40, 0.3Y‐LZNO) were carefully designed. The ionic conductivity of these PEO‐based HSEs were studied, and their performance in solid‐state lithium‐ion batteries with LiFePO4 (LFP) as cathode material and Li metal as anode were evaluated. The results showed that the HSE with addition content of inorganic powders, namely PEOLiTFSI@5 % GN‐LLZO +5 %0.3Y‐LZNO (noted as PL3) showed the optimized ionic conductivity of 2.9×10−4 S cm−1 at room temperature with an activation energy Ea of 0.21 eV. It has an electrochemical stability window of 4.65 V and ionic transfer number of 0.242. The addition of inorganic powders not only enhanced the ionic conductivities of PEO‐based HSEs, but also exhibited superior stability and interfacial compatibility with electrodes, leading to the improved cycle stability in the LFP/PL3/Li solid‐state battery configuration.

Sustainable cottonseed protein bioplastics: Physical and chemical reinforcement, and plant seedling growth application

Petroleum-based plastic containers for plant seedling growth are expensive to recycle and have negative environmental impacts when discarded. In this work, a novel family of sustainable and biodegradable plastic films and containers were fabricated by simply casting and mold-curing methods, which demonstrated outstanding performance promoting crop seed germination and plant seedling growth. Concentrate cottonseed protein (CPC) was used as polymeric matrix, pulp fiber (PF) as a physical reinforcement, tannic acid (TA) as a chemical modifying agent, with their addition contents ranging from 0 ∼ 30 % (PF) and 0 ∼ 10 % (TA), respectively. Evaluations of the composite CPC/PF and CPC/TA films regarding their structure, morphology, tensile properties, and water resistance show that the physical and chemical reinforcement resulted in good interfacial compatibility, mechanical strength, and water resistance. Moreover, the newly prepared bioplastics were biodegradable in soil in three weeks, and did not harm crop seed germination and growth. More importantly, the protein derived biocontainers/pot (CPC/PF30 and CPC/TA10) can provide excellent growth conditions for plant root and leaf growth such as chili peppers because of their low toxicity and 100 % germination rate. More importantly, the healthy growing environment was closely related to the presence of nutritious elements/ions that the plant needed. Specifically, the biodegradation of the bioplastics during plant seedling test released nitrogen-containing ions like NH4+ (0.25 wt% for CPC/TA10 versus 0.17 wt% for polyethylene), and retained in soil, playing a decisive role in seedling growth. Therefore, the cottonseed protein bioplastics reinforced by pulp fiber and tannic acid are beneficial to crop seedling growth, holding great potential for being used as plantable pots/containers in agriculture and horticulture applications.

Polyimide-coated MgO nanoparticles improves high-temperature energy storage performance in polyetherimide-based nanocomposite films

Enhancing the energy storage capacity of dielectric polymers can be achieved by the introduction of inorganic nanoparticles. However, the difference in surface energy often influences the interfacial compatibility of nanoparticles with polymers, consequently limiting their comprehensive dielectric properties. Here, the magnesium oxide (MgO) nanoparticles were coated with polyimide (PI) shells via in-situ polymerization, which is beneficial to improve the scattered particles in the polyether imide (PEI) matrix. The PI buffer shell is tightly bound to the PEI matrix through automatic electrostatic interaction making the defects decrease, together with the increased dielectric permittivity (εr) attributed to MgO, significantly enhancing the discharged energy density (Udis) and storage efficiency (η) of the PI@MgO/PEI nanocomposite films in harsh conditions. Thus, the maximal Udis of the PI@MgO/PEI nanocomposites is 4.33 J/cm3 at 150 °C, twice that of the pristine PEI. Even if an η exceeds 90 %, the Udis of 3.83 J/cm3 of 1 vol%-PI@MgO/PEI at 500 MV/m and 150 °C is better than that of the most advanced dielectric polymers.

Structure designing, interface engineering, and application prospects for sodium‐ion inorganic solid electrolytes

AbstractAll‐solid Na‐ion batteries (ASNIBs) present significant potential for integration into large‐scale energy storage systems, capitalizing on their abundant raw materials, exemplary safety, and high energy density. Among the pivotal components propelling the advancement of ASNIBs, inorganic solid electrolytes (ISEs) have garnered substantial attention in recent years due to their high ionic conductivity (σ), wide electrochemical stability window (ESW), and high shear modulus. Herein, this review systematically encapsulates the latest strides in Na‐ion ISEs, furnishing a comprehensive panorama of various ISE systems along with their interface engineering strategies against the electrodes. The prime focus resides in accentuating key strategies for refining ion conduction properties and interfacial compatibility of ISEs through structure design and interface modification. Furthermore, the review explores the foremost challenges and prospects inherent to sodium‐ion ISEs, striving to deepen our understanding of how to engineer more robust and efficient ISEs and interface stability, poised for the forthcoming era of advanced ASNIBs.

Solvent-Activated Transformation of Polymer Configurations for Advancing the Interfacial Reliability of Perovskite Photovoltaics.

Organic materials have been widely used as the charge transport layers in perovskite solar cells due to their structural versatility and solution processability. However, their low surface energy usually causes unsatisfactory thin-film wettability in contact with the perovskite solution, which limits the interfacial performance of the photovoltaic devices. Although solvent post-treatment could occasionally regulate the wetting behavior of organic films, the mechanism of the solid-liquid interaction is still unclear. Here, we present evidence of a possible correlation between the solvent and the wettability of a conventional polymer, poly[bis(4-phenyl) (2,4,6-trimethylphenyl) amine] (PTAA), and reveal the critical roles of Hansen solubility parameters (HSPs) of solvents in wetting mechanisms. Our results suggest that the conventional solvent N,N-dimethylformamide (DMF) improves the wettability of PTAA by the morphological disruption mechanism but negatively impacts interfacial charge collection and stability. In contrast, 2-methoxyethanol (2-Me) with an appropriate HSP value induces the transformation of the PTAA configuration in an orderly manner, which simultaneously improves the wetting property and maintains the film topography. After careful optimization of the surface conformation of the PTAA film, both perovskite crystallization and interfacial compatibility have been enhanced. Benefiting from superior interfacial properties, the perovskite solar cells based on 2-Me deliver a champion efficiency of 24.15% compared to 21.4% for DMF-based ones. More encouragingly, the use of 2-Me minimizes the perovskite buried interfacial defects, enabling the unencapsulated devices to maintain about 95% of their initial efficiencies after light illumination for 1100 h. The present study demonstrates the high effectiveness of solvent-polymer interaction for adjusting interfacial properties and strengthening the robustness of perovskite solar cells.

Lithium Phosphorous Oxynitride as an Advanced Solid‐State Electrolyte to Boost High‐Energy Lithium Metal Battery

AbstractLithium phosphorous oxynitride (LiPON) as one of the most successful solid‐state electrolytes (SSEs), has attracted great interest both in academia and technology due to its exceptional interfacial compatibility, broad electrochemical stability window, and excellent thermal stability, which enables the realization of extremely stable electrolyte/electrode interphase toward high‐energy density solid‐state lithium‐metal batteries (SSLMBs). However, insufficiency in ionic diffusion, mechanical robustness, and interfacial stability hinder its commercialization process. Herein, the characteristics of amorphous structure LiPON, fundamental understanding on the bulk ionic diffusion and electrode/electrolyte interface are systematically discussed, and the improvement strategies to boost the electrochemical performance are highlighted. Then, innovative characterization and computational methods help to unravel the design principle of LiPON are summarized. Furthermore, the approaches to realize high‐efficient preparation of LiPON are analyzed, followed by the investigation of present application of LiPON in current batteries. Finally, remaining challenges associated with the fundamental understanding and rational prediction of structure and interface design, high efficient preparation, and potential opportunities for future application of LiPON are properly prospected.

Preparation, mechanical properties and anti-oxidation behavior of lightweight porosity-controlled SiC(rGO, xZrB2) composite PDCs for thermal protection

Achieving well-balanced light weight with simultaneous improvement in mechanical and antioxidant properties of SiC-based composite polymer-derived ceramics (PDCs) for hypersonic vehicle components is still a huge challenge. Herein, lightweight SiC(rGO, xZrB2) composite PDCs were prepared via re-pyrolyzing ball-milling-induced ZrB2-SiC(rGO)p/polycarbosilane-vinyltriethoxysilane-graphene (PCS-VTES-GO, PVG) blends. Main reinforcements consist of ZrB2, ZrO2(ZrC), ZrOSi and SiO2/β-SiC phases, among which favorable compatibility enables enhanced bear loading performances and high-temperature oxidation resistance. Rigid SiC(rGO)p tightly links with flexible PVG pyrolysis products, and co-assembles into robust SiOxCy/Cfree(rGO) matrix in framework owing to plentiful Si-dangling bonds at their interfaces. More interestingly, interfacial ZrOSi/ZrC transition zone can augment structural disorder of ceramic network, give bridging effects, strengthen interfacial compatibility, and even hinder further crack propagation for self-densification. Particularly, SiC(rGO, 30%ZrB2) composite PDCs possess optimal hardness (6.49 GPa) and outstanding fracture toughness (5.77 MPa⋅m1/2). Porous SiC(rGO, 30%ZrB2) composite PDCs own stable structure integrity within 60-min testing under butane torch flame at 1300 °C. Self-healing protective SiO2-ZrO2 glass layer avoids destructive structure and timely covers defects, thus retains good mechanical performances. Such good synergistic reinforcement and multiscale design of porosity-controlled composite, realizes integration of lightweight/good load-bearing characteristics with improved oxidation resistance for thermal protection system (TPS) of hypersonic vehicles.

Flexible hexagonal boron nitride@liquid metal/polydimethylsiloxane composites with excellent thermal conductivity and superior mechanical properties

AbstractHexagonal boron nitride (h‐BN) has a layered lattice structure, high intrinsic thermal conductivity, and good chemical stability, and it has a promising applications in thermal management materials. However, poor interfacial compatibility and dispersion of BN flakes in the polymer matrix cause thermal contact resistance and gaps, directly impairing the performance of the composites and limiting their thermal conduction applications. Herein, the P‐BN@LM/PDMS thermally conductive composites with superior mechanical properties were fabricated by incorporating dopamine and liquid metal (LM) into BN flakes. The dopamine self‐polymerizes to form polydopamine (PDA) on the BN surface, denoted as P‐BN, which effectively improves interface compatibility and dispersion. The LM attaches to the functionalized P‐BN surface by mechanical grinding, acting as a bridge between adjacent BN flakes to enhance the integrity of the thermal conductive network within the composites. The coordination between P‐BN and LM increases interface strength, effectively improving mechanical performance. Hence, the P‐BN@LM/PDMS composites exhibit excellent thermal conductivity (4.0 W/mK) and an enhancement factor of 1373%, which is 2.22 times that of BN/PDMS composites with the same 30 wt% loading. Additionally, the composite shows superior tensile strength (2.11 MPa) and elongation at break (121%), representing 441% and 203% improvements compared with pure polydimethylsiloxane (PDMS). The P‐BN@LM/PDMS composites, with significant advantages in thermal conductivity and mechanical properties, are promising for future applications as flexible thermal interface materials in thermal management.Highlights The P‐BN@LM/PDMS composites exhibit excellent thermal conductivity (4.0 W/mK) and an enhancement factor of 1373%, making them promising for future applications as flexible thermal interface materials in thermal management. The P‐BN@LM/PDMS composites present a superior tensile strength (2.11 MPa) and elongation at break (121%). PDA formed by the self‐polymerization of dopamine on the BN surface effectively enhances interfacial compatibility and dispersion. LM attaches to the functionalized BN surface through mechanical grinding, acting as a bridge between adjacent BN flakes, thus enhancing the integrity of the thermal conductive network within the composites.

LLZTO crosslinks form a highly stretchable self-healing network for fast healable all-solid lithium metal batteries

Flexible composite solid electrolytes (CSEs) show great potentials in high-energy all-solid-state lithium metal batteries owing to their easy fabrication, good electrochemical properties, and high safety. However, it remains challenging to achieve good interfacial compatibility between the inorganic fillers and polymer matrix, which affects the lithium-ion transport efficiency and electrochemical performances of CSEs. Herein, a dynamic crosslinked network with Li6.4La3Zr1.4Ta0.6O12 (LLZTO) nanoparticles as the cross-linking point is proposed for fabrication of a rapidly self-healing flexible CSE, which is signed as SHENE. The amino groups in the 3-aminopropyltriethoxysilane modified LLZTO behave as the bridge sites to react with the copolymer of 2-hydroxyethyl methacrylate-g-4-formylbenzoic acid and poly (ethylene glycol) methoxy acrylate to form imine bonds, which effectively connect the organic/inorganic interface. Compared to the traditional physical contact, the covalent imine bonds can not only enhance the interaction between the two phases, but also improve the dispersion of the ceramic LLZTO nanoparticles. Additionally, the dynamic reversibility of imine bonds allows for enhanced mechanical strength and self-repairing capabilities of SHENE. Therefore, a Li||Li symmetrical cell assembled with SHENE can stably cycle for 5000 h at 0.05 mA cm−2 and 25 °C. The corresponding Li/SHENE/LiFePO4 full battery also exhibits good rate performance under various C-rates. Additionally, the Li/SHENE/LFP pouch cell exhibits superior safety under various abuse conditions. Therefore, this work provides new ideas for the uniform dispersion of ceramic nanoparticles in CSEs by the facile design of forming dynamic crosslinked networks.

Deciphering and Integrating Functionalized Side Chains for High Ion‐Conductive Elastic Ternary Copolymer Solid‐State Electrolytes for Safe Lithium Metal Batteries

AbstractA critical challenge in solid polymer lithium batteries is developing a polymer matrix that can harmonize ionic transportation, electrochemical stability, and mechanical durability. We introduce a novel polymer matrix design by deciphering the structure‐function relationships of polymer side chains. Leveraging the molecular orbital‐polarity‐spatial freedom design strategy, a high ion‐conductive hyperelastic ternary copolymer electrolyte (CPE) is synthesized, incorporating three functionalized side chains of poly‐2,2,2‐Trifluoroethyl acrylate (PTFEA), poly(vinylene carbonate) (PVC), and polyethylene glycol monomethyl ether acrylate (PEGMEA). It is revealed that fluorine‐rich side chain (PTFEA) contributes to improved stability and interfacial compatibility; the highly polar side chain (PVC) facilitates the efficient dissociation and migration of ions; the flexible side chain (PEGMEA) with high spatial freedom promotes segmental motion and interchain ion exchanges. The resulting CPE demonstrates an ionic conductivity of 2.19×10−3 S cm−1 (30 °C), oxidation resistance voltage of 4.97 V, excellent elasticity (2700 %), and non‐flammability. The outer elastic CPE and the inner organic–inorganic hybrid SEI buffer intense volume fluctuation and enable uniform Li+ deposition. As a result, symmetric Li cells realize a high CCD of 2.55 mA cm−2 and the CPE‐based Li||NCM811 full cell exhibits a high‐capacity retention (~90 %, 0.5 C) after 200 cycles.