Supramolecular Elastomers Research Articles

Mussel-inspired, fully biobased, mechanically robust, and room temperature healable supramolecular elastomer composites for sustainable strain sensors

The sustainable development of strain sensors necessitates the use of mechanically robust and self-healing elastomers derived from biobased feedstocks to ensure durability, extend service life, and reduce reliance on fossil resources. Herein, we report mussel-inspired, fully biobased, mechanically robust, room-temperature healable supramolecular elastomer composites (SECs) fabricated from natural rubber (NR), polydopamine (PDA), and cellulose nanofiber (CNF). Hydrogen bonds were formed among the hydroxyl and secondary amine groups of PDA, hydroxyl groups of CNF, and the non-rubber components of NR, resulting in room-temperature self-healing and mechanically reinforced NR/PDA/CNF SECs. The SECs achieved a tensile strength of up to 9.5 MPa and recovered over 80 % of its strength after self-healing at room temperature for 3 h. The robust adhesion properties of PDA within the SECs enabled the surface coating of the SECs with conductive carbon nanotubes (CNT) to fabricate flexible strain sensors without additional adhesives through a simple dip-coating technique. These flexible strain sensors exhibited excellent structural stability, high sensitivity, and reliability, making them suitable for human motion signal detection. This study underscores the potential of biobased and self-healing elastomers in enhancing the performance and sustainability of flexible strain sensors, contributing significantly to the development of sustainable and durable sensing technologies.

Li+ Ion-Dipole Interaction-Enabled a Dynamic Supramolecular Elastomer Interface Layer for Dendrite-Free Lithium Metal Anodes.

The unstable lithium (Li)/electrolyte interface, causing inferior cycling efficiency and unrestrained dendrite growth, has severely hampered the practical deployment of Li metal batteries (LMBs), particularly in carbonate electrolytes. Herein, we present a robust approach capitalizing on a dynamic supramolecular elastomer (DSE) interface layer, which is capable of being reduced with Li metal to spontaneously form strong Li+ ion-dipole interaction, thereby enhancing interfacial stability in carbonate electrolytes. The soft phase in the DSE structure enables fast Li+ transport via loosely coordinated Li+-O interaction, while the hard phase, rich in electronegative lithiophilic sites, drives the generation of fast-ion-conducting solid electrolyte interface components, including Li3N and Li2S. Furthermore, the dynamically resilient DSE network composed of soft and hard phases protects Li anodes from electrolyte corrosion and accommodates volume changes during cycling. All features of the DSE layer synergistically facilitate uniform Li+ deposition and suppress Li dendrite propagation, ensuring a stable and dendrite-free Li anode. Consequently, the symmetric Li||Li cell incorporating the DSE layer achieves cycling stability exceeding 6000 h under 1 mA cm-2 and 1 mA h cm-2 conditions. Furthermore, full cell pairing DSE/Li anode with LiFePO4 (LFP) or high-voltage LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes exhibits high-efficiency Li deposition and cycling stability, even under constrained conditions of limited Li (40 μm) and ultrahigh loading NMC811 cathode (21.5 mg cm-2). This study underscores the effectiveness of the ion-dipole interaction-enabled DSE network in developing stable, high-energy-density LMBs.

Supramolecular Cross-Linked High-Performance Self-Healing Elastomers toward Wearable Sensing Applications

Supramolecular Cross-Linked High-Performance Self-Healing Elastomers toward Wearable Sensing Applications

Hierarchical H-bonding and metal coordination bonds enabled supramolecular dual networks for high-performance energy-dissipation

Natural organisms have superior material properties such as mechanical adaptability, impact protection, and self-healing to protect the body from complicated external environments, fascinating the development of functional supramolecular elastic materials with biomimetic protective features. Herein, a dual physically crosslinked supramolecular polyurethane (PU) network with strain-hardening effect is synthesized by incorporating hierarchical hydrogen bonds (H-bond) and metal coordination bonds into an elastomer matrix. A moderate content of quadruple H-bonds is critical for achieving a prominent toughness and a considerable strain-at-break owing to the strain hardening effect enabled by the hierarchical H-bonds. When the Zn-to-pyridine coordination bonds were introduced to the supramolecular PU, the strength, toughness, and energy dissipation properties were further enhanced attributing to the dual physical crosslinking networks. The dynamic dissociation and association of the sacrificial H-bonds and Zn-to-pyridine coordination bonds induced significant strain hardening effect and enabled tremendous energy absorption and self-healing properties. Besides, the supramolecular PU elastomers and their blends were foamed via scCO2 foaming to produce supramolecular foams containing dynamic bonds. The composite foam could effectively reduce the impact force from 6085 N to 373 N and achieve an outstanding energy absorption efficiency of 93.87% owing to the synergistic effect of porous structure and dual physically crosslinked networks. This work provides an innovative strategy for designing high-performance energy absorbing supramolecular elastomers and cushioning foams with reversible bonds.

3D printing of lignin-based supramolecular topological shape-morphing architectures with high strength, toughness, resolution, and fatigue resistance

The design and fabrication of customized and sustainable elastomers with supramolecular frameworks remain a central focus of scientific research. 3D printing represents an advanced manufacturing technology that has garnered significant attention. Lignin, a naturally abundant polymer, fits well with 3D printing due to its unique aromatic-rich structures that can provide rigidity and structural support. However, challenges persist in developing UV-curable lignin-based inks and fabricating high-strength lignin-based composite hydrogels with tailored shapes and structures through vat photopolymerization (VPP) printing techniques, largely due to lignin’s inherent heterogeneity, fragility, and poor fluidity. Here, we successfully developed a unique lignin-based photosensitive macromonomer resin tailored for VPP 3D printing. Using an ethanol/water fractionation process, heterogeneous lignosulfonate (LS), a by-product of the pulp and paper industry, was treated to isolate highly reactive lignin fractions rich in phenolic hydroxyl and sulfonic groups. These fractions were then chemically modified to synthesize a lignin-based macromonomer known as urethane acrylated lignosulfonate (UALS). The resulting lignin-based macromonomer (15–35 wt%) exhibits excellent compatibility with photosensitive resin formulations, enabling effective VPP 3D printing. The 3D-printed lignin-based supramolecular composite hydrogels exhibit high strength (tensile strength of ∼2.12 MPa, an elongation at break of ∼220.13 %), high resolution, fatigue resistance (up to 10000 cycles), and moisture-induced responsive behavior. The development of 3D-printed lignin-based supramolecular elastomers with defined shapes and patterned structures significantly advances the discovery of robust and environmentally sustainable soft materials with potential applications in soft robotics and tissue engineering.

Mechanically customizable lignin bio-elastomers based on tailorable multiscale microstructures

The development of bio-based polyurethanes (PU) elastomers with well-designed multiscale microstructures to customize their mechanical performances was desired, but remained an ongoing challenge. Herein, a novel strategy of integrating tailorable hard-soft nanophases with multiple hydrogen bond (H-bond) interactions was proposed to construct mechanically customizable PU bio-elastomers. In this strategy, highly reactive lignin with high hydroxyl contents was employed as bio-polyol monomer reacting with hexamethylene diisocyanate (HDI) to construct carbamate bonds with a function of tailoring H-bond degree via altering the feeding ratio of lignin. The rigid lignin cooperating with HDI as hard segments self-assembled to generate phase separated nanostructures. Consequently, the integration of well-defined hard-soft nanophases and multiple H-bond interactions in the synthesized lignin-based PU (LPU) achieved excellent and customizable mechanical performances ranging from highly elastic rubber to highly stiff plastic with ultrahigh strength of 72.8 MPa and unprecedented modulus of 3.5 GPa. Impressively, rubber-like LPU elastomers could recover 90 % of initial stress even after 500 stretching cycles, indicating fascinating resilience and fatigue resistance. More especially, rigid LPU plastics with fully hard domains and dense H-bond networks could be transformed into flexible and bendable paper-like elastomers once eliminating intermolecular H-bond interactions under 60 °C hot water. Thus, this work provides a feasible and promising approach to construct supramolecular PU elastomers with excellent and customizable mechanical performances to extend their on-demand applications.

Gelatin-strengthened elastomer derived from polymerizable deep eutectic solvent for soft ionotronics

It is widely recognized that resolving the trade-off between mechanical toughness and recyclability in elastomers presents a significant challenge. This study introduces a novel gelatin-strengthened, supramolecular cross-linked elastomer (PCCA-G) synthesized through in situ photo-polymerization of a polymerizable deep eutectic solvent (PDES) system composed of choline chloride and acrylic acid. The research highlights the dual benefits of integrating gelatin into the PDES system in the absence of covalent cross-linker, notably enhancing mechanical properties and recycle ability. The PCCA-G3 % elastomers demonstrate exceptional transparency with a transmittance of 95.4 %, robust mechanical strength (approximately 4.99 MPa), and substantial strain capacity (1169 %). These properties make the elastomers ideal for loading-bearing sensor applications, capable of monitoring various human motions with high accuracy and sensitivity. Furthermore, the elastomers exhibit outstanding recycle properties via a simple solvation-evaporation process, maintaining performance after multiple cycles. This work addresses the critical need for environmental-friendly materials potentially reducing the ecological impact of widespread sensor usage. The adaptable nature of these materials also positions them as promising candidates for future developments in sensor technology and soft ionotronics.

Biomass and Transparent Supramolecular Elastomers for Green Electronics Enabled by the Controlled Growth and Self-Assembly of Dynamic Polymer Networks.

Determining the optimal method for preparing supramolecular materials remains a profound challenge. This process requires a combination of renewable raw materials to create supramolecular materials with multiple functions and properties, including simple fabrication, sustainability, a dynamic nature, good toughness, and transparency. In this work, a strategy is presented for toughening supramolecular networks based on solid-phase chain extension. This toughening strategy is simple and environmentally friendly. In addition, a series of biobased elastomers are designed and prepared with adjustable performance characteristics. This strategy can significantly improve the transparency, tensile strength, and toughness of the synthesized elastomer. The synthesized biobased elastomers have great ductility, repairability, and recyclability, and they show good adhesion and dielectric properties. A biobased ionic skin is assembled from these biobased elastomers. Assembled ionic skin can sensitively detect external stimuli (such as stretching, bending, compression, or temperature changes) and monitor human movement. The conductive and dielectric layers of the biobased ionic skin are both obtained from renewable raw materials. This research provides novel molecular design approaches and material selection methods for promoting the development of green electronic devices and biobased elastomers.

Highly flexible and transparent self-healing elastomer based on localized supramolecular interactions with enhanced mechanical properties and long-term storage stability

This study prepared a highly flexible and transparent self-healing elastomer with enhanced mechanical properties and long-term storage stability, facilitated by localized supramolecular interactions. By incorporating a functional oligomer containing localized urea groups into a conventional elastomeric matrix, increased supramolecular interactions were promoted through multiple hydrogen bonds among clustered functional groups. The resulting supramolecular elastomers exhibited excellent optical properties, including total transmittance exceeding 90 %, yellow index less than 2, and haze under 1 %, along with elastic recovery of 40 %. Notably, the self-healing elastomer developed in this study effectively overcame the typical trade-off between mechanical and self-healing properties in conventional self-healing materials, achieving superior mechanical strengths compared to conventional elastomers and an outstanding self-healing efficiency of 94.0 % within a few minutes. Moreover, by tailoring the chemical structure of the oligomer, significant improvements in the long-term solution storage stability of the solution for urea systems were achieved. These results are attributed to the unique supramolecular network derived from multiple hydrogen bonding interactions among the localized functional groups in a confined zone. A mechanism for improved mechanical properties and outstanding self-healing performance is also proposed using a model system.

Autonomous Underwater Self-Healable Adhesive Elastomers Enabled by Dynamical Hydrophobic Phase-Separated Microdomains.

High-efficient underwater self-healing materials with reliable mechanical attributes hold great promise for applications in ocean explorations and diverse underwater operations. Nevertheless, achieving these functions in aquatic environments is challenging because the recombination of dynamic interactions will suffer from resistance to interfacial water molecules. Herein, an ultra-robust and all-environment stable self-healable polyurethane-amide supramolecular elastomer is developed through rational engineering of hydrophobic domains and multistrength hydrogen bonding interactions to provide mechanical and healing compatibility as well as efficient suppression of water ingress. The coupling of hydrophobic chains and hierarchical hydrogen bonds within a multiphase matrix self-assemble to generate dynamical hydrophobic hard-phase microdomains, which synergistically realize high stretchability (1601%), extreme toughness (87.1MJm-3), and outstanding capability to autonomous self-healing in various harsh aqueous conditions with an efficiency of 58% and healed strength of 12.7MPa underwater. Furthermore, the self-aggregation of hydrophobic clusters with sufficient dynamic interactions endows the resultant elastomer with effective instantaneous adhesion (6.2MPa, 941.9Nm-1) in extremely harsh aqueous conditions. It is revealed that the dynamical hydrophobic hard-phase microdomain composed of hydrophobic barriers and cooperative reversible interactions allows for regulating its mechanical enhancement and underwater self-healing efficiency, enabling the elastomers as intelligent sealing devices in marine applications.

Dynamic‐Bond‐Mediated Chain Reptation Enhances Energy Dissipation of Elastomers

AbstractVibrations with various frequencies in daily life and industry can cause health hazards and fatigue failure of critical structures, which requires the development of elastomers with high energy dissipation at desired frequencies. Current strategies relying on tuning characteristic relaxation time of polymer chains are mostly qualitative empirical methods, and it is difficult to precisely control damping performances. Here, we report a general strategy for constructing dynamic crosslinked polymer fluid gels that provide controllable ultrahigh energy dissipation. This is realized by dynamic‐bond‐mediated chain reptation of polymer fluids in a crosslinked network, where the characteristic time of chain reptation is dominated by the presence of well‐defined dissociation time of dynamic bonds and almost independent of their molar mass. Using prototypical supramolecular polydimethylsiloxane elastomers, we demonstrate that dynamic crosslinked polymer fluid gels exhibit a controllable ultrahigh damping performance at desired frequencies (10−2~102 Hz), exceeding that of typical state‐of‐the‐art silicone damping materials. Their shock absorption is over 300 % higher than that of commercial silicone rubber under the same impact force.

Dynamic-Bond-Mediated Chain Reptation Enhances Energy Dissipation of Elastomers.

Vibrations with various frequencies in daily life and industry can cause health hazards and fatigue failure of critical structures, which requires the development of elastomers with high energy dissipation at desired frequencies. Current strategies relying on tuning characteristic relaxation time of polymer chains are mostly qualitative empirical methods, and it is difficult to precisely control damping performances. Here, we report a general strategy for constructing dynamic crosslinked polymer fluid gels that provide controllable ultrahigh energy dissipation. This is realized by dynamic-bond-mediated chain reptation of polymer fluids in a crosslinked network, where the characteristic time of chain reptation is dominated by the presence of well-defined dissociation time of dynamic bonds and almost independent of their molar mass. Using prototypical supramolecular polydimethylsiloxane elastomers, we demonstrate that dynamic crosslinked polymer fluid gels exhibit a controllable ultrahigh damping performance at desired frequencies (10-2~102 Hz), exceeding that of typical state-of-the-art silicone damping materials. Their shock absorption is over 300 % higher than that of commercial silicone rubber under the same impact force.

Robust, self-healing AIE fluorescent supramolecular elastomers for smart anti-counterfeiting

Providing aggregation-induced emission (AIE) polyurethane with self-healing capability can increase the lifetime of the material and adapt it to multiple application scenarios, which is a huge challenge in the development of luminescent smart materials. Herein, a range of transparent fluorescence polyurethanes (FPUs) with prominent strength were designed and synthesized. The optimization of robust FPUs exhibits outstanding mechanical performance (33.5 MPa tensile strength, 120.2 MJ m−3 toughness) and self-healing ability (88.9 %, at 80 °C for 2 h). Furthermore, the aggregation of tetraphenylethylene structure in the hard segment causes the system to emit bright blue fluoresence. We successfully screen-printed designable patterns on the self-healing polyurethane substrates. The concealed patterns self-repair after damage, and can be clearly and robustly displayed under 365 nm light irradiation. The as-prepared multifunctional self-healing material, exhibiting stable AIE fluorescence, is anticipated to possess significant value in the domains of smart anti-counterfeiting materials, flexible display screens and intelligent optoelectronics.

Application of Multilayered Blend Films as Soft, Stretchable, Self‐Adhesive, and Self‐Healing Absorption‐Dominant EMI Shielding and Microwave Absorber

AbstractSolution‐processable organic conductor–supramolecular elastomer blends are emerging materials for intrinsically stretchable and autonomously self‐healing organic electronics. Herein, the feasibility of a heterogenous multiphase polymer blend is demonstrated for soft, ultraflexible, self‐adhesive, and self‐healing multilayered film structures for electromagnetic interference (EMI) shielding and microwave absorber (MWA) purposes. The developed soft multilayered films achieve a 5–40 fold improvement in the thickness of the MWA compared to the current state‐of‐the‐art. The thickness normalized reflection loss (RL) is up to 65.26 dB mm−1 with 8.5 GHz bandwidth at 18–26.5 GHz. The maximum thickness normalized EMI shielding effectiveness peaks at up to 175 dB mm−1. The EMI shielding and MWA properties are maintainable up to 150% tensile strain with only a small decrease in the overall attenuation and RL. Furthermore, the developed films are capable of fully autonomously self‐healing and achieve a tough adhesion in temperatures of −30–145 °C, and underwater with maximum single‐lap shear adhesion strength of ≈481.5 kPa to soft thermoplastic polyurethane films. Thus, the developed multilayered films can be utilized for absorption‐dominant EMI shielding or MWA purposes as stretchable coatings. The developed materials also show considerable potential for emerging damage and puncture‐resistant organic soft electronics with autonomous material‐level self‐healing.

Supramolecular elastomers with high strength and low toxicity are suitable for safety protection

Elastomer with high strength and toughness, temperature resistance and low smoke toxicity have shown great application prospects in the field of safety protection. In order to meet the needs of high strength, high toughness and smoke toxicity safety, a high-strength structural elastomer is formed by introducing the integration of hard skeleton and soft elastomer, that is, two-dimensional black phosphorus with high flame retardant efficiency and bimetallic hydroxide with catalytic detoxification (BP-MA-LDH) as the hard skeleton, based on the special combination of internal hydrogen bonds. High strength supramolecular poly(Urethane) (SPU) elastomer was manufactured by molecular design. The high strength and toughness SPU elastomer also has a tensile strength of 53.77 Ma and a elongation at break of 715.26 %. The addition of 2.0 wt% BP-MA-LDH reduces the heat release rate of SPU by 58.84 % and the smoke production release by 61.54 %. In terms of flue gas toxicity inhibition, Fractional Effective Dose was used to evaluate the flue gas toxicity of elastomer composites, and the release of CO, HCN, oxynitride and other toxic gases were greatly reduced. The synthetic performance of SPU elastomer composites in strengthening and toughening, smoke suppression and toxicity reduction is much better than that reported by peers.

Mechanical Stretch α-Cyclodextrin Pseudopolyrotaxane Elastomer with Reversible Phosphorescence Behavior.

Polyethylene glycol chains in two terminals of the naphthalene functional group are threaded into α-cyclodextrin cavities to form the pseudopolyrotaxane (NPR), which not only effectively induces the phosphorescence of the naphthalene functional group by the cyclodextrin macrocycle confinement, but also provides interfacial hydrogen bonding assembly function between polyhydroxy groups of cyclodextrin and waterborne polyurethane (WPU) chains to construct elastomers. The introduction of NPR endows the elastomer with enhanced mechanical properties and excellent room temperature phosphorescent(RTP) emission (phosphorescence remains in water, acid, alkali, and organic solvents, even at 160 °C high temperatures). Especially, the reversible mechanically responsive room temperature phosphorescence behavior (phosphorescence intensity increased three times under 200% strain) can be observed in the mechanical stretch and recover process, owing to strain-induced microstructural changes further inhibiting the non-radiative transition and the vibration of NPR. Therefore, changing the phosphorescence behavior of supramolecular elastomers through mechanical stretching provides a new approach for supramolecular luminescent materials.

Flexible Cages Enable Robust Supramolecular Elastomers.

Advances in modern industrial technology continue to place stricter demands on engineering polymeric materials, but simultaneously possessing superior strength and toughness remains a daunting challenge. Herein, a pioneering flexible cage-reinforced supramolecular elastomer (CSE) is reported that exhibits superb robustness, tear resistance, anti-fatigue, and shape memory properties, achieved by innovatively introducing organic imide cages (OICs) into supramolecular networks. Intriguingly, extremely small amounts of OICs make the elastomer stronger, significantly improving mechanical strength (85.0MPa; ≈10-fold increase) and toughness (418.4MJm-3; ≈7-fold increase). Significantly, the cooperative effect of gradient hydrogen bonds and OICs is experimentally and theoretically demonstrated as flexible nodes, enabling more robust supramolecular networks. In short, the proposed strengthening strategy of adding flexible cages effectively balances the inherent conflict between material strength and toughness, and the prepared CSEs are anticipated to be served in large-scale devices such as TBMs in the future.

Low hysteresis zwitterionic supramolecular polymer ion-conductive elastomers with anti-freezing properties, high stretchability, and self-adhesion for flexible electronic devices.

The fabrication of stretchable ionic conductors with low hysteresis and anti-freezing properties to enhance the durability and reliability of flexible electronics even at low temperatures remains an unmet challenge. Here, we report a facile strategy to fabricate low hysteresis, high stretchability, self-adhesion and anti-freezing zwitterionic supramolecular polymer ion-conductive elastomers (ICEs) by photoinitiated polymerization of aqueous precursor solutions containing a newly designed zwitterionic monomer carboxybetaine ureido acrylate (CBUIA) followed by solvent evaporation. The resultant poly(carboxybetaine ureido acrylate) (PCBUIA) ICEs are highly stretchable and self-adhesive owing to the presence of strong hydrogen bonds between ureido groups and dipole-dipole interactions of zwitterions. The zwitterion groups on the polymer side chains and loaded-lithium chloride endow PCBUIA ICEs with excellent anti-freezing properties, demonstrating mechanical flexibility and ionic transport properties even at a low temperature (-20 °C). Remarkably, the PCBUIA ICEs demonstrate a low hysteresis (≈10%) during cyclic mechanical loading-unloading (≤500%), and are successfully applied as wearable strain sensors and triboelectric nanogenerators (TENGs) for energy harvesting and human motion monitoring. In addition, the PCBUIA ICE-based TENG was used as a wireless sensing terminal for Internet of Things smart devices to enable wireless sensing of finger motion state detection.

Thermomechanically stable supramolecular elastomers inspired by heat shock proteins.

Supramolecular polymers are usually thermomechanically unstable, as their mechanical strength decreases drastically upon heating, which is a fatal shortcoming for their application. Herein, inspired by heat shock proteins (HSPs) which enable living organisms to tolerate lethal high temperatures, we design an HSP-like response to impart a supramolecular elastomer with high thermomechanical stability. The HSP-like response relies on the reversible hydrolysis of boronic acid and the tunable association strength of boron dative bonds. As the temperature increases, the boronic acid dehydrates and transforms into boroxane. The boroxane, acting as a heat shock chemical, prevents the disintegration of the supramolecular network through formation of multiple and stronger dative bonds with imidazole-containing polymers, thereby enabling the material to retain its mechanical strength at high temperatures. Such chemical transformation and network change induced by the HSP-like response are fully reversible during the heating and cooling processes. Moreover, due to the dynamic nature of the supramolecular network, the elastomer possesses recycling and self-healing abilities.

Building Ion-Conductive Supramolecular Elastomeric Protective Layer via Dynamic Hard Domain Design for Stable Zinc Metal Anodes.

The instability of zinc metal anode caused by zinc dendrite growth and severe parasitic reactions has significantly restricted the extensive application of rechargeable aqueous zinc-ion batteries (RAZBs). Herein, based on the strategy of dynamic hard domains, we develop an ion-conductive supramolecular elastomer consisting of Zn salts and the polyurethane-urea-polypropylene glycol polymer skeleton. This elastomer combines high mechanical strength, high ionic conductivity, decent hydrophobicity, and high adhesion to stabilize the electrode-electrolyte interface. In the elastomer system, this elastomer can dynamically adapt to the volume changes of Zn anodes during repeated zinc plating/stripping processes through the reversible dissociation/reassociation of hierarchical hydrogen bonds (H-bonds) formed by the polar groups of urea and urethane moieties. Meanwhile, the coordination of Zn2+ with soft polypropylene glycol (PPG) segments contributes to fast ion transport. This hydrophobic elastomer can also effectively inhibit water-induced corrosion by shielding the active Zn metal from the aqueous electrolyte. Based on the above synergies, the surface-modified anode shows excellent cycling stability above 550 h at a high current density of 5 mA cm-2 and a capacity of 2.5 mAh cm-2. Moreover, the assembled Zn//MnO2 full cell also displayed an enhanced electrochemical performance. This work provides inspiration for the design of solid electrolyte interphase (SEI) layers in aqueous battery chemistry to accelerate the application of RAZBs.