Cascade reactions have garnered considerable attention owing to their high efficiency, operational simplicity, and compliance with green chemistry principles. Pickering emulsion with a large reaction interface provides a good platform but remains challenging, such as achieving spatial isolation of distinct catalytically active sites within the emulsion system. Janus nanosheets with asymmetric structures offer an ideal solution to this issue. Herein, ionic liquid-functionalized Janus nanosheets (Janus-IL) were synthesized and subsequently combined with poly(N-isopropylacrylamide) (PNIPAM) to act as emulsifiers for stabilizing Pickering emulsions. Remarkably, the phase behavior of the Pickering emulsion exhibits reversible alternation between emulsification and demulsification upon temperature switching between 25 degrees C and 40 degrees C, demonstrating excellent temperature responsiveness. Based on the temperature-switchable emulsion micro-reactor stabilized by the synergistic effect of Janus-IL and PNIPAM, a cascade reaction was successfully carried out, which not only shortened the reaction time and reduced the temperature, but also achieved the coupling of product separation and emulsifier recycling.
Water scarcity affects the survival of over 2.2 billion people worldwide, emerging as a pressing global challenge. Atmospheric water harvesting based on porous adsorbents presents a promising solution to this crisis. However, the current adsorption materials exhibit quite low capturing capacity under extremely low atmospheric humidity. Herein, we synthesized a class of M-gallate (M = Mg, Co, and Ni) metal-organic frameworks (MOFs) and evaluated their atmospheric water harvesting performance. Impressively, Mg-gallate MOF was stable for at least 28 days in water, and exhibited exceptional water uptake capacity of 170.0 mg/g at 0.2% relative humidity (RH) and 178.6 mg/g at 2.6% RH, which exceeds the highest value of the previously reported porous materials under the same conditions. Even at 5.0% RH, its water adsorption capacity is lower than that of the record-breaking water-stable Ni2Cl2BBTA. Spectral studies and DFT calculations suggest that the water adsorption process follows a multi-layer mechanism. The main driving forces underlying the outstanding atmospheric water harvesting performance of the MOF are the hydrogen bonding interactions between water molecules and the oxygen-containing functional groups (carboxylate and phenolic-OH) in MOF framework, the hydrogen bonding among adsorbed water molecules, and the synergistic effect of pore filling. Thus, the strategy developed here provides a simple and effective way for the development of high-performance atmospheric water adsorbents under ultra-low humidity environments.
Aqueous zinc-ion batteries (AZIBs) exhibit tremendous application potential in cutting-edge interdisciplinary fields such as wearable devices and biomedicine owing to their high safety, low cost, excellent electrochemical performance, and good biocompatibility. This paper provides a systematic review of structural-engineering strategies and recent advances in their gel electrolytes, with particular emphasis on the integrated optimization of ionic conduction, biocompatibility, mechanical properties, and interfacial stability of hydrogel and polymer electrolytes guided by molecular engineering and interfacial regulation. Furthermore, the development potential and evolution trends of hydrogel electrolytes in flexible integration and biomedical applications are discussed. This research provides novel ideas for the design and expanded application of high-performance hydrogel electrolytes.
Energy storage devices are crucial components of modern energy systems, playing a vital role in driving industrial development and facilitating societal progress. Among various candidates, iron-ion hybrid supercapacitors (IIHSs) have attracted considerable attention as a next-generation energy storage technology, owing to their ability to combine the charge-storage mechanisms of both batteries and supercapacitors. In this work, we report the synthesis of a flexible Fe3+/Cu2+ dual-doped MnO2 electrodes based on carbon cloth (FeCuMnO2@CC) featuring nanospheres and tailored physicochemical properties through a one-step hydrothermal treatment. Under the synergistic regulation of Fe3+ and Cu2+, the physical adsorption kinetics process of Fe2+ is effectively accelerated. Moreover, the introduction of ascorbic acid into the Fe2+ electrolyte effectively suppressed spontaneous oxidation, thereby enhancing electrochemical stability. Benefiting from these design strategies, the resulting aqueous IIHS demonstrated an exceptional areal capacitance of 970.83 mF cm-2 at a current density of 1 mA cm-2 (809 F g-1 at 0.8333 A g-1) and maintained 74.75 % of its initial capacitance after 20,000 charge-discharge cycles. In addition, the assembled flexible device maintained 58.9 % of its capacitance after 10,000 cycles under mechanical deformation. These findings not only highlight the potential of MnO2-based electrodes for application in iron-ion energy storage systems but also offer valuable insights into advancing flexible and high-performance iron-ion energy storage devices.
Increasing the cut-off voltage of the LiCoO2 (LCO) cathode holds great promise for achieving high-energy-density lithium metal batteries. However, at cut-off voltages above 4.5 V, issues such as interfacial instability and transition metal dissolution severely hinder practical application. Here, we report a quasi-solid-state electrolyte (PCA) constructed from 2-cyanoethyl acrylate (CA) units, which promotes the formation of a high-quality cathode electrolyte interface (CEI) by regulating the composition and structure of the electric double layer (EDL). CA preferentially adsorbs onto LCO surfaces and coordinates with Co ions, stabilizing the cathode structure, while its strong ion-dipole interactions with DFOB-anions promote co-accumulation within the inner Helmholtz plane (IHP), excluding solvent molecules to construct a stable and dense organic-inorganic hybrid CEI. Benefiting from this, the Li|PCA|LCO battery retains 84 % of its capacity after 600 stable cycles at a high cutoff voltage of 4.6 V and also exhibits excellent performance in full cells with high-loading cathodes and pouch cells. Furthermore, by increasing the cut-off voltage, the assembled pouch cell achieves a high energy density of 433.6 Wh kg-1. This work highlights the critical role of polymers in regulating the EDL/IHP structure and offers a new approach for the development of high-voltage quasi-solid-state lithium metal batteries.
A complexation-chelation strategy stabilizes the four-electron redox for aqueous zinc–bromine batteries by complexing polybromides at the cathode and chelates Zn 2+ at the anode, endowing the cells with superior energy density and cycling durability.
Aqueous zinc-iodine batteries (AZIBs) emerge as a highly promising electrochemical energy storage technology due to their inherent safety, environmental and friendliness low cost. However, the inherent challenges including polyiodide shuttle effect, zinc dendrite growth and side reactions prevent their practical applications. This work proposes an innovative "sword and shield" strategy to simultaneously resolve the above issues, through the simple addition of 1,3,5-trioxane (TXE) to a common ZnSO4 aqueous electrolyte. The TXE acts as a molecular "sword" that disrupts SO4 2--H2O coordination, directly preventing the formation of contact ion pairs and optimizing the solvation structure of Zn2+. The restructured solvation sheath selectively excludes SO42-, raises the desolvation energy barrier, and promotes the formation of a stable solid electrolyte interphase on Zn anode. Consequently, water activity is significantly suppressed, the formation of by-products is effectively inhibited, and uniform Zn deposition is achieved. Moreover, the TXE center dot SO42 aggregates function as a "shield." They establish an electrostatic repulsion barrier that blocks I3 shuttling, while accelerating the conversion kinetics of I3 /I . The TXE-modified AZIBs deliver a high specific capacity of 195 mAh g-1 at 0.3 A g-1, excellent rate capability and superior cycling stability (96.3% capacity retention after 50,000 cycles). And the pouch cell also maintains stable operation for over 520 cycles. This facile and effective synergistic optimization strategy provides new insight into designing high-safety and long-life aqueous halide batteries.
Multifunctional carbon fiber structural batteries simultaneously provide mechanical load-bearing and energy storage capabilities, offering significant potential to replace conventional structural components, thereby enhancing the overall energy density of the system. However, achieving high multifunctional efficiency remains challenging, as lithium-ion transport in carbon fibers is restricted at high current densities, resulting in poor rate capability and significantly decreased reversible capacity. To solve this problem, this work develops an integrated structural anode of carbon/carbon composite (C/C) for both structural support and energy storage. Atomic force microscopy combined with in situ characterization techniques, including in situ Fiber Bragg Grating sensing, in situ electrochemical impedance spectroscopy, and Operando Raman spectroscopy, reveals that the unique "onion-skin" buffering structure in C/C significantly enhances the mechano-electrochemical properties of the electrode through a synergistic "shielding-channeling" mechanism. The all-fiber structural lithium-ion battery with commercial organic electrolyte demonstrates a high energy density of 60 Wh kg-1 with excellent power density (65 W kg-1) and cycling stability. Remarkably, it achieves a record-high near-unity multifunctional efficiency (0.96), while maintaining remarkable electrochemical stability under tensile, bending and out-of-plane compressive conditions, demonstrating great potential for applications in aerospace systems, intelligent transportation, and next-generation lightweight structural energy storage technologies.
Low-temperature environments significantly affect the performance of lithium metal batteries, primarily due to the freezing of commercial electrolytes that induced increased energy barriers for lithium-ion migration and desolvation, unstable solid electrolyte interphases (SEI), and lithium dendrite growth. In this work, an electrolyte was developed with lithium nitrate as an additive and lithium bis(trifluoromethanesulfonyl)imide and lithium hexafluorophosphate as the main lithium salts. Li+-NO3- coordination weakens Li+-solvent binding, enabling anion penetration into solvation shells. This multianion-dominated structure promotes Li+ diffusion/desolvation kinetics while enabling inorganic-rich SEI formation and homogeneous Li deposition. Consequently, Li||Li cells exhibit exceptional stability across -30 to 25 °C with over 2000 h cycle life. Li||NCM811 cells demonstrate outstanding rate capability at 25 °C, retaining 94.7% capacity at 2 C and 85.1% at 5 C over 1000 cycles. Notably, under cryogenic conditions at 0.2 C and -30 °C, the cell achieves 92.4% capacity retention after 400 cycles.
Aqueous zinc-bromine batteries (AZBBs) gain considerable attention as a next-generation energy storage technology due to their high energy density, cost-effectiveness and intrinsic safety. Despite these advantages, challenges such as the polybromide ion shuttle effect, self-discharge, and zinc anode instability hinder their widespread applications. This review provides a comprehensive and systematic examination of recent advancements in AZBBs, beginning with an in-depth discussion of the fundamental electrochemical mechanisms underlying bromine redox reactions and the principal challenges inherent to these systems. Subsequently, it elucidates the most recent developments in the fabrication and optimization of electrode materials, electrolytes and separators, with particular emphasis on innovative strategies to ameliorate existing limitations. Furthermore, this article delineates the persisting challenges and prospective research directions for advancing AZBBs, including the design of advanced cathode materials, electrolyte optimization and device engineering. By addressing these critical aspects, this work endeavors to provide valuable insights and guidance for the development of high-performance AZBBs, paving the way for their practical implementation in large-scale energy storage applications.
Solid-state batteries (SSBs) promise to revolutionize energy storage by offering enhanced safety, higher energy density, and improved cycle lifespan over conventional lithium-ion batteries. Among the various solid electrolytes, polymers stand out for their unique combination of processability, mechanical compliance, and chemical versatility. This review explores why polymers are poised to lead the race toward commercial SSBs. Their intrinsic advantages-such as superior interfacial contact with electrodes, tunable ionic conductivity, and compatibility with scalable manufacturing methods-as well as the key technical challenges they face, including limited thermal stability, narrow electrochemical windows, and interfacial degradation, are examined. This study highlights emerging solutions from recent research, including polymer molecular design, polymer-ceramic composites, and in situ polymerization strategies. In contrast to oxide and sulfide systems, which face significant barriers in cost, manufacturability, and integration, polymer-based electrolytes offer a realistic and economically viable path to large-scale deployment. With continuing advances in materials design and industrial processing, polymers are not only competitive-they are leading the transition to next-generation solid-state batteries.
The rapid evolution of wearable and portable electronics has created a critical demand for innovative energy solutions that combine sustainability with mechanical flexibility. Self-charging systems have become one of the most promising solutions; enhancing their adaptability and intelligence is key for further application. Here, we present a novel self-charging system that integrates a direct-current triboelectric nanogenerator (DC-TENG) with an electrochromic supercapacitor through a compatible electrode, demonstrating both flexibility and self-powering capabilities. For DC-TENG, single-walled carbon nanotubes (SWCNTs) are doped with small organic molecules to prepare the P/N-type semiconductor fabric. The tribovoltaic phenomenon arising from interfacial sliding between the two types of fabric enables direct current generation through mechanical motion. Additionally, P-type fabric is applied as the compatible electrode to combine with a uniform PB film for a flexible all-solid-state supercapacitor, which can serve as the flexible energy storage component for wearable electronic devices. As a result, the flexible power system constructed with these components enables self-charging motion sensing and allows real-time monitoring of the charging process through color changes. This work effectively simplifies the structure of self-charging systems and opens up new potential applications for the development of multifunctional and intelligent systems.
Commercial lithium-ion batteries that use flammable liquid electrolytes face significant safety risks, such as fires caused by electrolyte leaks. Solid polymer electrolytes (SPEs) present a viable solution to this problem, with ether-based polymer electrolytes standing out due to their superior stability and compatibility with lithium metal. The in situ ring-opening polymerization of cyclic ether monomers not only simplifies the battery manufacturing process but also improves the solid/solid interfacial contacts between electrolytes and electrodes, thereby significantly reducing interfacial impedance. In this paper, we review the mechanisms of ring-opening polymerization for cyclic ether monomers and analyze the ionic conduction of ether-based polymer electrolytes. We also explore the in situ curing mechanisms for several representative cyclic ether monomers and assess research advancements in this area. Additionally, this paper discusses the sustainability of ether-based polymer electrolytes and provides an outlook on future research and sustainability initiatives in the field.
Aqueous zinc-iodine batteries (AZIBs) are promising for cost-effective energy storage. However, some critical problems related to the slow reaction kinetics of iodine conversion, polyiodide shuttle effect and polyiodide corrosion greatly hinder their practical applications. Herein, a novel bipyridine-based nonporous covalentorganic cage (Bpd-COC) is developed as a high-performance cathode for AZIBs with active electrolyte containing I-/I3- redox couple. The rapid I-/I3- conversion mechanism involved in the Bpd-COC cathode and the strong intermolecular host-guest interactions between Bpd-COC and I3- are revealed by comprehensive in-situ/ex-situ experimental characterizations and theoretical calculations. The Bpd-COC selectively captures I3- ions through electron-pair interactions between the framework nitrogen atoms and the adsorbed I3- ions, thus the shuttle of I3- is effectively suppressed. Consequently, the AZIB with Bpd-COC cathode achieves a high specific capacity of 197.3 mAh g-1 at 0.3 A g-1, excellent rate capability (110.9 mAh g-1 retained at 5 A g-1), and superior cycling stability (over 40,000 cycles with 93.5 % capacity retention). Moreover, the corrosion of the Zn metal anode normally triggered by the polyiodide shuttling is significantly alleviated. This work paves a promising avenue for the development of intrinsically safe, high-rate and long-lifespan AZIBs.
While iron-ion hybrid capacitors (IIHCs) represent the advantages of high theoretical specific capacity, low cost, and environmental friendliness, their high charge density tends to cause structural degradation in conventional electrode materials, resulting in impaired cycling stability and reduced capacitive performance. To address this issue, this work proposes a flexible Co2+ doped V2O5 cathode via a hydrothermal method to achieve highperformance IIHCs. The Co2+ doping enhances the crystalline stability of V2O5 while creating a distinctive hierarchical morphology. Meanwhile, through simulations, we analyzed the adsorption energy of the Co2+ doped V2O5 cathode, revealing that this optimized structure promotes efficient kinetics for iron-ion intercalation/ deintercalation and enhances ionic transport pathways. When implemented as a cathode material, the Co-V2O5 composite achieves an areal capacitance of 1200 mF cm(-2) at 1 mA cm(-2). Notably, the device maintains 93.7 % capacitance retention after 5000 charge-discharge cycles, showcasing remarkable cycling durability. In addition, a quasi-solid flexible device using PVA-FeCl2 as an electrolyte was assembled, which delivers a high surface capacitance of 639 mF cm(-2) at 1 mA cm(-2), with the long-term durability of 80 % of the capacitance retention rate. These findings not only validate the effectiveness of transition metal doping in stabilizing vanadium-based frameworks but also highlight the feasibility of developing high-performance IIHCs for next-generation energy storage applications.
Zinc-ion hybrid supercapacitors (ZIHSCs) have garnered widespread attention due to their integration of the excellent characteristics of both batteries and capacitors. This study employs a synergistic strategy combining hydrothermal and high-temperature calcination methods to construct a nanosphere-structured T-Nb2O5 composite anode material coated with reduced graphene oxide (rGO) on a flexible carbon cloth (CC) substrate (T-Nb2O5/rGO@CC), in conjunction with a hierarchical super-mesoporous activated carbon cathode (ACcp@CC) derived from discarded citrus peel. The rGO coating structure suppresses the volume expansion of the internal nanostructure caused by charging and discharging, effectively enhancing mechanical stability. At the same time, the three-dimensional conductive network of rGO effectively compensates for the poor intrinsic conductivity of Nb2O5. The constructed ZIHSC delivers a capacitance of 718.56 mF cm-2 at 1 mA cm-2, and achieves a maximum energy density of 399.20 mu Wh cm-2 at 1 mW cm-2. Furthermore, after 50,000 ultralong-cycle, the capacity retention rate is 104.17 %. The assembled flexible device not only possesses excellent mechanical properties but also delivers a specific capacitance of 389.89 mF cm-2 at 1 mA cm-2, providing long-term power for various electronic devices. This study provides a solid theoretical reference for the design of stable composite structures and the investigation of ultra-long cycling performance in niobium-based electrode materials.
Structural batteries are an emerging class of multifunctional electrochemical energy storage devices that combine mechanical load-bearing capabilities with energy storage. These batteries aim to address the weight and volume efficiency challenges faced by conventional batteries, particularly in electric vehicles, thereby extending driving range. As a crucial component of structural batteries, the electrolyte must not only facilitate ion transport but also provide mechanical integrity under flexural loads or impacts. However, developing a structurally strong electrolyte is a significant challenge, as high mechanical strength often leads to reduced ionic conductivity. Therefore, the full potential of structural batteries can only be realized once suitable multifunctional structural electrolytes are developed. This review examines the state-of-the-art in structural electrolytes, focusing on thermoplastic and thermoset polymer-based electrolytes for structural batteries. It explores the underlying ion transport mechanisms and mechanical enhancement strategies. The review also discusses how electrolyte composition—such as the choice of polymer matrix, inorganic fillers, solvents, and ionic liquid additives—affects both mechanical and electrochemical properties, as well as the role of interfacial stability. Furthermore, block copolymer electrolytes and molecular ion composite solid electrolytes based on rigid-rod polymers are proposed as promising candidates for structural electrolytes. The article also addresses the challenges and future prospects for these materials, aiming to provide insights into overcoming the limitations of polymer-based electrolytes with high mechanical strength, thus promoting their practical application in structural batteries.
Lithium metal batteries often generate substantial heat during operation due to persistent side reactions between the lithium metal anode and the electrolyte. Without effective regulation, this heat accumulation can lead to catastrophic thermal runaway. Here, an intelligent thermal regulation system based on a stimuli‐responsive poly(pentafluoropropyl acrylate) (PPFA) matrix is reported that precisely controls the release of LiDFOB via temperature‐dependent ion‐dipole interactions. Under normal operating conditions, strong PPFA‐DFOB − ion‐dipole interactions immobilize anions and facilitate the in situ formation of a robust solid electrolyte interphase, enabling Li||LiFePO 4 cells to achieve exceptional cycling stability over 500 cycles with 78.3% capacity retention at 1C. Under thermal abuse, the system dynamically switches to favor DOL‐DFOB − coordination, triggering the release of DFOB − and initiating 1,3‐dioxolane (DOL) polymerization, which results in a 34‐fold reduction in parasitic heat generation. This smart transition significantly improves safety metrics, achieving elevated self‐heating and thermal runaway onset temperatures of 108 and 286 °C, respectively, in 1.5 Ah pouch cells. This work establishes a new paradigm of molecular‐level thermoregulation via ion–dipole interaction control, offering a promising strategy for the development of inherently safer and high‐performance lithium metal batteries.
Dual-carbon potassium-ion hybrid capacitors (PIHCs) offer the potential to deliver cost-effectiveness, extended cycle durability, high energy and power densities. Nevertheless, their widespread implementations are significantly restricted by the sluggish kinetics of conventional carbon-based anodes. Herein, nitrogen-sulfur co-doped carbon nano-onions (NS-CNOs) are introduced as advanced anode materials for dual-carbon PIHCs. The unique architecture of NS-CNOs characterized by concentric graphitic layers with moderate specific surface area and suitable interlayer spacing, not only effectively mitigates the stress variations induced by repeated K+ insertion/ extraction but also enhances K+ storage capability. The synergies of N, S co-doping expand the interlayer spacing of graphene, introduce abundant potassiophilic sites/defects, and establish efficient ion/electron transport pathways. Through a combination of in/ex-situ experimental characterizations and theoretical simulations, it is demonstrated that K+ ions are preferentially adsorbed at the N-sites during potassiation process, and S atoms provide additional defects for K+ extraction. These advantages contribute to excellent rate performance (100 mAh g- 1 at 20 A g- 1) and good cycling stability for NS-CNOs. When integrated into dual-carbon PIHCs, the device enables high energy and power densities (174.4 Wh kg- 1 and 14.0 kW kg- 1) while maintaining long-term cycling stability (86.7 % capacity retention after 10,000 cycles). This work explores a potential design strategy of anode materials for high-performance dual-carbon PIHCs.
Short-circuits induced by Zn dendrite growth and external impacts can lead to the failure of aqueous zinc-ion batteries (AZIBs). To enhance the mechanical safety of aqueous batteries, most of the work focuses on strengthening the external packaging, while comparatively limited attention has been directed toward the properties and optimization of the internal electrolyte. Herein, a smart multifunctional fluid [polymethyl methacrylate dispersed in Zn(OTf)2 aqueous solution] is developed as both a highly ionic conductive electrolyte and an intrinsic mechanical protector for AZIBs. This electrolyte exhibits dynamic "liquid-solid" interconversion due to its non-Newtonian fluid properties. Under normal circumstances, the fluid's high ionic conductivity (25.2 mS cm-1) supports efficient electrochemical kinetics and interfacial compatibility. Upon high current rates or sudden external impacts, the electrolyte stiffens to suppress Zn dendrite growth and prevent internal short circuits. An AZIB (Zn||V6O13) using this electrolyte achieves a specific capacity of 353.6 mAh g-1 at 0.1 A g-1, good rate capability (206.9 mAh g-1 at 5 A g-1), and excellent cyclability with 85 % capacity retention after 3000 cycles at 5 A g-1. Additionally, the electrolyte's shear-thickening effect ensures stable operation of the cell under impacts. This work highlights the dual functionality of the electrolyte in enhancing both electrochemical performance and mechanical safety in AZIBs.