Jul 2026· Advances in Materials· pp.
e74011
· 0 citations· 146 references
Medicine
Abstract
Dynamic polymers, featuring reversible networks enabled by dynamic covalent bonds or non-covalent interactions, exhibit functionalities such as self-healing, reprocessability, mechanical adaptability, and recyclability. These attributes offer innovative material platforms to address critical challenges in next-generation high-performance lithium-based batteries (LBBs), including unstable solid-solid interfaces, the trade-off between mechanical robustness and ionic conductivity, and battery sustainability. This review summarizes recent advances in the design strategies, working mechanisms, and electrochemical performance of dynamic polymers for three major fields of LBBs: polymer electrolyte design, interface engineering, and binder development. By summarizing the relationships among dynamic bond chemistry (e.g., hydrogen bonds, disulfide, boronate ester, and imine bonds), network dynamics, and functional performance, we highlight the unique roles of dynamic polymers in improving interfacial stability, suppressing lithium dendrite growth, accommodating electrode volume changes, and enabling closed-loop recycling of battery components. Finally, we outline existing challenges and future research directions of the application of dynamic polymers toward the realization of high-energy-density, long-cycle-life, safe, and sustainable LBBs, providing insightful perspectives for the rational design of smart and eco-friendly battery materials.
Lithium metal batteries (LMBs) hold great promise for next-generation high-energy-density energy storage, yet their practical deployment is severely hindered by lithium dendrite growth, unstable solid electrolyte interphase (SEI), infinite volume expansion of lithium anodes, and poor thermal safety. As an abundant, renewable, biodegradable, and low-cost biomass polymer, cellulose and its derivatives feature outstanding mechanical robustness, tunable flexibility, rich surface hydroxyl groups, and designable hierarchical micro/nanostructures, which endow them with unique advantages in addressing critical bottlenecks of LMBs. This review focuses on the multifunctional roles and underlying mechanisms of cellulose-based composites in boosting the electrochemical and safety performance of LMBs. By virtue of polar functional groups and rigid-flexible integrated structures, cellulose can effectively homogenize Li+ flux, guide uniform lithium deposition, suppress dendrite nucleation and propagation, and alleviate volume fluctuation during cycling. Meanwhile, cellulose-based matrices significantly enhance the mechanical strength, thermal stability, flame retardancy, and ionic conductivity of polymer electrolytes and separators. Seven types of functional cellulose composites are highlighted regarding their applications in electrolytes, separators, 3D anode hosts, artificial interphase layers, and interface regulators. Finally, the future development of cellulose materials toward high-performance LMBs is prospected from the aspects of precise molecular modification, biomimetic ordered ion transport, and scalable green fabrication. This review provides systematic insights into the performance enhancement mechanisms and application strategies of cellulose for high-safety and long-lifespan lithium metal batteries.
Jun Guan, Minxin Wang, Zihao Zheng et al.· Advances in Materials· 1 citation
Organic materials are highly promising to construct Aluminum (Al)-organic batteries (AOBs) due to their low-cost, sustainability, and structural flexibility. However, key challenges like high solubility and over-reliance on conductive additives largely constrain their implementation. Herein, we propose a conjugated ladder polymer, poly(benzimidazo-benzophenanthroline) (BBL), as a stable cathode for durable AOBs. The rigid skeleton from a double-stranded fused-ring structure and extensive π-π intermolecular interactions endow BBL with insolubility and fast charge transfer kinetics. With moderate addition of carbon nanotubes (20%) in the electrode, the freestanding BBL cathode exhibits impressive cycling stability and rate performance under a wide range of temperatures (-20°C-100°C). Specifically, the BBL electrode delivers a reversible capacity of 117 mAh/g and stable cycling over 10000 cycles, as well as an excellent anti-self-discharge behavior. A series of characterizations confirmed AlCl2 + as the charge carrier and C═O groups of BBL as the redox active sites. Interestingly, without any form of energy input, a room-temperature self-charging function is also noticed with at most 82% capacity self-charged. Our work highlights the significance of advanced structure design for Al-organic batteries.
Qing Lang, Jiahui Ye, Jiayuan Yu et al.· Small· 0 citations
Lithium metal batteries are severely hindered by interfacial instability issues such as dendrite growth, unstable solid electrolyte interphase, and volume expansion. Crystalline dynamic covalent frameworks have emerged as a promising class of artificial solid electrolyte interphase materials to address these challenges, owing to their unique combination of reversible bond chemistry and ordered pore architectures. This synergy enables these frameworks to homogenize Li+ flux, suppress dendrite penetration, accommodate volume changes, and even impart self-healing capabilities. This review provides a comprehensive overview of recent advances in crystalline dynamic covalent frameworks for lithium anode protection, organized according to four representative dynamic covalent linkages: imine, boronate ester, N→B dative, and disulfide bonds. This review systematically discusses key design principles, including lithophile site engineering, pore structure, dynamic bond chemistry utilization, and framework processability. Finally, this review points out the current challenges and looks ahead to future directions, including multi-dynamic hybrid frameworks, the design of processable solutions, machine learning to accelerate discovery, and intelligent stimulus-response interfaces, all aimed at inspiring the development of high-performance lithium metal anode protective layers.
Aqueous zinc-ion batteries (AZIBs) have garnered significant attention due to their high safety, environmental friendliness, and remarkable cost-effectiveness. However, developing cathode materials with strong structural stability and long cycle life remains a critical challenge. Herein, chitosan-doped HNaV6O16·4H2O (HNVC) is synthesized via a hydrothermal process with chitosan incorporation to optimize the material’s nanostructure. Unlike conventional polymer doping, chitosan introduction exhibits behavior analogous to metal-ion intercalation, effectively stabilizing the layered framework. As a result, HNVC delivers remarkable cycling durability and maintains a capacity retention rate of 95.5% after 8500 cycles at 5 A g−1. Comprehensive electrochemical and spectroscopic analyses reveal that chitosan-assisted regulation reduces the interlayer spacing and enables a synergistic Zn2+/H+ co-intercalation mechanism, contributing to both enhanced capacity and structural robustness. This work provides a strategy for polymer-assisted structural engineering of vanadate-based cathodes toward high-performance AZIBs.
Jinqiang Huang, Yan Ran, Xu Li et al.· ACS Applied Energy Materials· 0 citations
Dynamic polymer networks (DPNs), constructed via reversible covalent bonds or non-covalent interactions, have emerged as a versatile material platform that uniquely combines stimuli-responsive adaptability, reprocessability, and recyclability with the mechanical robustness of thermosets. These attributes have recently become particularly attractive for thermal management applications, where conventional static materials often suffer from single functionality, poor interfacial adaptability, and end-of-life non-recyclability. This perspective provides a systematic overview of recent advances in DPN-based thermal management materials, organized around three technological pathways: switchable thermal conductivity materials, adaptive thermal interface materials, and dynamic radiative cooling materials. We discuss how reversible bond exchange enables molecular-level regulation of chain conformation, filler network architecture, and interfacial conformability, thereby achieving on-demand control of heat transport, reduction of contact thermal resistance, and dynamic modulation of radiative cooling performance. The intrinsic recyclability of DPNs further allows material repair, reshaping, and component recovery, supporting circular economy principles. Finally, we identify key challenges-including the trade-off between dynamicity and long-term stability, response speed, multifunctional integration, and scalable manufacturing-and offer perspectives on future directions toward intelligent, sustainable, and high-performance thermal management systems.
Jiajia Yang, Ziman Zheng, Xinhong Xiong et al.· Macromolecular rapid communi...· 0 citations
This review systematically summarizes recent advances in employing thermoresponsive polymers to address the challenges of interfacial instability and thermal runaway in aqueous zinc-ion batteries (AZIBs), which are promising candidates for safe, low-cost energy storage. The discussion focuses on three innovative regulatory strategies: self-healing electrolytes that autonomously repair interfacial defects through reversible sol-gel transitions; intelligent shutdown mechanisms that rapidly block ion transport at a threshold temperature to prevent thermal runaway; and robust electrolyte systems that maintain performance under extreme conditions by preserving physical integrity and optimizing ion solvation. The established correlation between gel-phase behavior and battery failure mechanisms provides a novel design framework for developing AZIBs with high safety and long cycle life. Finally, future perspectives highlight the need for a rational design framework that links stimuli-responsive behavior to performance, paving the way for the predictive design of adaptive hydrogel systems.
Xiaohui Pan, Xiaoqin Liu· Small· 0 citations
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