Search Results (21)

The promise of lithium–oxygen batteries lie not merely in their record-breaking theoretical energy density, but in the challenge of making such energy truly reversible. Rising as the key obstacle is the lithium metal anode, whose remarkable capacity and low potential come at the cost of dendritic growth, unstable solid electrolyte interphases, and relentless reactions with oxygen species. These instabilities, once overshadowed by cathode-related limitations, now define the frontier of research as current densities and energy demands approach practical levels. This review highlights recent progress in two complementary directions for anode protection: physical approaches, such as artificial protective layers, solid or functional separators, and oxygen-blocking interlayers that isolate and stabilize the surface; and chemical strategies, including electrolyte and additive design that enable in situ formation of LiF- and Li₃N-rich interfaces with high ionic conductivity and chemical robustness. Together, these approaches establish a unified framework for achieving dendrite-free and oxygen-resistant lithium interfaces. Mastering solid electrolyte interfacial stability rather than only cathode catalysis will ultimately determine whether lithium oxygen battery can evolve from laboratory prototypes to truly viable high-energy systems. Full article

Silicon is widely recognized as a next-generation anode owing to its exceptional theoretical capacity, yet its practical deployment in lithium-ion batteries is constrained by severe volume expansion, particle fracture, loss of electrical percolation, and solid electrolyte interphase layer instability. Polymer-based strategies have emerged as accessible solutions to engineer extensive volume changes and interfacial compatibility, while preserving pathways for charge transport. Viscoelastic polymer binders dissipate stress, catechol-inspired chemistries strengthen adhesion and tailor interphases, and conductive polymers can function simultaneously as binder, electronic additive, and artificial SEI. This review describes these approaches through a structure–process–performance perspective, emphasizing practically relevant metrics, such as initial capacity, initial Coulombic efficiency, and long-term cycling stability. We organize the main section into (i) dopamine-derived interfacial engineering, (ii) self-healing three-dimensional network binders, and (iii) conductive-polymer-based designs. In the last section, we articulate the functional requirements of polymers in silicon anodes, outline the ideal structural designs, and provide forward-looking avenues for future lithium-ion battery anode research. Full article

MXene–polymer hybrids combine the high in-plane conductivity and rich surface chemistry of MXenes with the processability and mechanical tunability of polymers for lithium-metal and lithium–sulfur batteries. Most reported systems still rely on HF-etched MXenes, introducing F-rich terminations, safety and waste issues, and poorly controlled surfaces. This review instead centers on fluoride-free synthesis routes, benchmarks them against HF methods, and translates route–termination relationships into practical rules for choosing polymer backbones. We track the evolution from early linear hosts such as PEO- and PVDF-type polymers to polar nitrile or carbonyl matrices, crosslinked and ionogel networks, and emerging biopolymers and COF-type porous frameworks that are co-designed with MXene terminations to regulate ion transport, interfacial chemistry, and mechanical robustness. These chemistry–backbone pairings are linked to five scalable fabrication modes, including solution blending and film casting, in situ polymerization, surface grafting, layer-by-layer assembly, and electrospinning, and to roles as solid or quasi-solid electrolytes, artificial interphases, separator-like coatings, and electrode-facing architectures. Finally, we highlight key evidence gaps and reporting standards needed to de-risk scale-up of green MXene–polymer batteries. Full article

Metal anodes promise improvements in energy density and cost; however, their performance is determined within the first several nanometers at the interface. This review reports on how polymer-based artificial solid electrolyte interphases (SEIs) are engineered to stabilize Li and aqueous-Zn anodes, and how these designs are now evaluated against operando readouts rather than post-mortem snapshots. We group the related molecular strategies into three classes: (i) side-chain/ionomer chemistry (salt-philic, fluorinated, zwitterionic) to increase cation selectivity and manage local solvation; (ii) dynamic or covalently cross-linked networks to absorb microcracks and maintain coverage during plating/stripping; and (iii) polymer–ceramic hybrids that balance modulus, wetting, and ionic transport characteristics. We then benchmark these choices against metal-specific constraints—high reductive potential and inactive Li accumulation for Li, and pH, water activity, corrosion, and hydrogen evolution reaction (HER) for Zn—showing why a universal preparation method is unlikely. A central element is a system of design parameters and operando metrics that links material parameters to readouts collected under bias, including the nucleation overpotential (η_nuc), interfacial impedance (charge transfer resistance (R_ct)/SEI resistance (R_SEI)), morphology/roughness statistics from liquid-cell or cryogenic electron microscopy (Cryo-EM), stack swelling, and (for Li) inactive-Li inventory. By contrast, planar plating/stripping and HER suppression are primary success metrics for Zn. Finally, we outline parameters affecting these systems, including the use of lean electrolytes, the N/P ratio, high areal capacity/current density, and pouch-cell pressure uniformity, and discuss closed-loop workflows that couple molecular design with multimodal operando diagnostics. In this view, polymer artificial SEIs evolve from curated “recipes” into predictive, transferable interfaces, paving a path from coin-cell to prototype-level Li- and Zn-metal batteries. Full article

Polymer materials have become promising candidates for next-generation energy storage, with structural tunability, multifunctionality, and compatibility with a variety of device platforms. They have a molecular design capable of customizing ion and electron transport routes, integrating redox-active species, and enhancing interfacial stability, surpassing the drawbacks of traditional inorganic systems. New developments have been made in multifunctional polymers that have the ability to combine conductivity, mechanical properties, thermal stability, and self-healing into a single scaffold system, which is useful in battery, supercapacitor, and solid-state applications. By incorporating polymers with carbon nanostructures, ceramics, or two-dimensional materials, hybrid polymer nanocomposites improve electrochemical performance, durability, and mechanical compliance, and the solid polymer electrolytes, as well as artificial solid electrolyte interphases, resolve dendrite growth and safety issues. The multifunctionality also extends to flexibility, stretchability, and miniaturization, which implies that polymers are suitable for use in wearable devices and biomedical devices. At the same time, sustainable polymer innovation focuses on bio-based feedstocks, which can be recycled, and green synthesis pathways. Polymer discovery using artificial intelligence and machine learning is faster than standard methods, predicts structure–property–performance relationships, and can be rationally engineered. Although there are difficulties in stability during long periods, scalability, and trade-offs between indeedness and mechanical endurance, polymers are a promising avenue with regard to dependable, safe, and sustainable power storage. This review presents the molecular strategies, multifunctional uses, and prospects, where polymers are at the center of the next-generation energy technologies. Full article

Solid-state lithium batteries (SSLBs) have emerged as a promising alternative to conventional lithium-ion systems due to their superior safety profile, higher energy density, and potential compatibility with lithium metal anodes. However, a major challenge hindering their widespread deployment is the formation and growth of lithium dendrites, which compromise both performance and safety. This review provides a comprehensive and structured overview of recent advances in dendrite suppression strategies, with special emphasis on the role played by the nature of the solid electrolyte. In particular, we examine suppression mechanisms and material innovations within the three main classes of solid electrolytes: sulfide-based, oxide-based, and polymer-based systems. Each electrolyte class presents distinct advantages and challenges in relation to dendrite behavior. Sulfide electrolytes, known for their high ionic conductivity and good interfacial wettability, suffer from poor mechanical strength and chemical instability. Oxide electrolytes exhibit excellent electrochemical stability and mechanical rigidity but often face high interfacial resistance. Polymer electrolytes, while mechanically flexible and easy to process, generally have lower ionic conductivity and limited thermal stability. This review discusses how these intrinsic properties influence dendrite nucleation and propagation, including the role of interfacial stress, grain boundaries, void formation, and electrochemical heterogeneity. To mitigate dendrite formation, we explore a variety of strategies including interfacial engineering (e.g., the use of artificial interlayers, surface coatings, and chemical additives), mechanical reinforcement (e.g., incorporation of nanostructured or gradient architectures, pressure modulation, and self-healing materials), and modifications of the solid electrolyte and electrode structure. Additionally, we highlight the critical role of advanced characterization techniques—such as in situ electron microscopy, synchrotron-based X-ray diffraction, vibrational spectroscopy, and nuclear magnetic resonance (NMR)—for elucidating dendrite formation mechanisms and evaluating the effectiveness of suppression strategies in real time. By integrating recent experimental and theoretical insights across multiple disciplines, this review identifies key limitations in current approaches and outlines emerging research directions. These include the design of multifunctional interphases, hybrid electrolytes, and real-time diagnostic tools aimed at enabling the development of reliable, scalable, and dendrite-free SSLBs suitable for practical applications in next-generation energy storage. Full article

In this work, graphite anodes and lithium iron phosphate (LFP) cathodes are used to examine the effects of sodium hexafluorophosphate (NaPF₆) and potassium hexafluorophosphate (KPF₆) electrolyte additives on the formation of the solid electrolyte interphase and the performance of lithium-ion batteries in both half-cell and full-cell designs. The objective is to assess whether these additives may increase cycle performance, decrease irreversible capacity loss, and improve interfacial stability. Compared to the control electrolyte (1.22 M Lithium hexafluorophosphate (LiPF₆)), cells with NaPF₆ and KPF₆ additives produced less SEI products, which decreased irreversible capacity loss and enhanced initial coulombic efficiency. Following the formation of the solid electrolyte interphase, the specific capacity of the control cell was 607 mA·h/g, with 177 mA·h/g irreversible capacity loss. In contrast, irreversible capacity loss was reduced by 38.98% and 37.85% in cells containing KPF₆ and NaPF₆ additives, respectively. In full cell cycling, a considerable improvement in capacity retention was achieved by adding NaPF₆ and KPF₆. The electrolyte, including NaPF₆, maintained 67.39% greater capacity than the LiPF₆ baseline after 20 cycles, whereas the electrolyte with KPF₆ demonstrated a 30.43% improvement, indicating the positive impacts of these additions. X-ray photoelectron spectroscopy verified that sodium (Na⁺) and potassium (K⁺) ions were present in the SEI of samples containing NaPF₆ and KPF₆. While K⁺ did not intercalate in LFP, cyclic voltammetry confirmed that Na⁺ intercalated into LFP with negligible impact on the energy storage of full cells. These findings demonstrate that NaPF₆ and KPF₆ are suitable additions for enhancing lithium-ion battery performance in the popular artificial graphite/LFP system. Full article

Recent advancements in lithium-metal-based battery technology have garnered significant attention, driven by the increasing demand for high-energy storage devices such as electric vehicles (EVs). Lithium (Li) metal has long been considered an ideal negative electrode due to its high theoretical specific capacity (3860 mAh g⁻¹) and low redox potential. However, the commercialization of Li-metal batteries (LMBs) faces significant challenges, primarily related to the safety and cyclability of the negative electrodes. The formation of lithium dendrites and uneven solid electrolyte interphases, along with volumetric expansion during cycling, severely hinder the commercial viability of LMBs. Among the various strategies developed to overcome these challenges, the introduction of artificial protective layers and the structural engineering of current collectors have emerged as highly promising approaches. These techniques are critical for regulating Li deposition behavior, mitigating dendrite growth, and enhancing interfacial and mechanical stability. This review summarizes the current state of Li-negative electrodes and introduces methods of enhancing their performance using a protective layer and current collector design. Full article

Lithium (Li) metal’s exceptional low electrode potential and high specific capacity for next-gen energy storage devices make it a top contender. However, the unregulated and unpredictable proliferation of Li dendrites and the instability of interfaces during repeated Li plating and stripping cycles pose significant challenges to the widespread commercialization of Li metal anodes. We introduce the creation of a hydrogen bond network solid electrolyte interphase (SEI) film that integrates zwitterionic groups, designed to facilitate the stability and longevity of lithium metal batteries (LMBs). Here, we design a PVA/P(SBMA-MBA) hydrogen bond network film (PSM) as an artificial SEI, integrating zwitterions and polyvinyl alcohol (PVA) to synergistically regulate Li⁺ flux. The distinctive zwitterionic effect in the network amplifies the SEI film’s ionic conductivity to 1.14 × 10⁻⁴ S cm⁻¹ and attains an impressive Li⁺ ion transfer number of 0.84. In situ Raman spectroscopy reveals dynamic hydrogen bond reconfiguration under strain, endowing the SEI with self-adaptive mechanical robustness. These properties facilitate a homogeneous Li flux and exceptionally suppress dendritic growth. The advanced Li metal anode may endure over 1200 h at 1 mA cm⁻² current density and 1 mAh cm⁻² area capacity in a Li|Li symmetric battery. And in full cells paired with LiFePO₄ cathodes, 93.8% capacity retention is reached after 300 cycles at 1C. Consequently, this work provides a universal strategy for designing dynamic interphases through molecular dipole engineering, paving the way for safe and durable lithium metal batteries. Full article

The increasing demand for high-specific-energy lithium batteries has stimulated extensive research on the lithium metal anode owing to its high specific capacity and low electrode potential. However, the lithium metal will irreversibly react with the electrolyte during the first cycling process, forming an uneven and unstable solid electrolyte interphase (SEI) layer, which results in the non-uniform deposition of Li ions and thus the formation of lithium dendrites. This could cause a battery short circuit, resulting in safety hazards such as thermal runaway. In addition, the continuous rupture and repair of the SEIs during the repeated charge/discharge processes will constantly consume the active lithium, which leads to a significant decrease in battery capacity. An effective strategy to address these challenges is to design and construct ideal artificial SEIs on the surface of the lithium metal anode. This review analyzes and summarizes the mathematical modeling of SEI, the functional characteristics of SEIs with different components, and finally discusses the challenges faced by artificial SEIs in practical applications of lithium metal batteries and future development directions. Full article

Li metal anodes could significantly improve battery energy density. However, Li generally electrodeposits in poorly controlled morphology, leading to safety and performance problems. One factor that controls Li anode performance and electrodeposition morphology is the nature of the electrolyte–current collector interface. Herein, we modify the Cu current collector interface by depositing precisely controlled nanoporous carbon (NPC) coatings using pulsed laser deposition to develop an understanding of how NPC coating density and thickness impact Li electrodeposition. We find that NPC density and thickness guide Li morphological evolution differently and dictate whether Li deposits at the NPC-Cu or NPC-electrolyte interface. NPC coatings generally lower overpotential for Li electrodeposition, though thicker NPC coatings limit kinetics when cycling at a high rate. Lower-density NPC enables the highest Coulombic efficiency (CE) during calendar aging tests, and higher-density NPC enables the highest CE during cycling tests. Full article

Aqueous zinc-ion batteries (AZIBs) have become a promising and cost-effective alternative to lithium-ion batteries due to their low cost, high energy, and high safety. However, dendrite growth, hydrogen evolution reactions (HERs), and corrosion significantly restrict the performance and scalability of AZIBs. We propose the introduction of a BaTiO₃ (BTO) piezoelectric polarized coating as an interface modification strategy for ZIBs. The low surface energy of the BTO (110) crystal plane ensures its thermodynamic preference during crystal growth in experimental processes and exhibits very low reactivity toward oxidation and corrosion. Calculations of interlayer coupling mechanisms reveal a stable junction between BTO (110) and Zn (002), ensuring system stability. Furthermore, the BTO (110) coating also effectively inhibits HERs. Diffusion kinetics studies of Zn ions demonstrate that BTO effectively suppresses the dendrite growth of Zn due to its piezoelectric effect, ensuring uniform zinc deposition. Our work proposes the introduction of a piezoelectric material coating into AZIBs for interface modification, which provides an important theoretical perspective for the mechanism of inhibiting dendrite growth and side reactions in AZIBs. Full article

Developing a reasonable design of a lithiophilic artificial solid electrolyte interphase (SEI) to induce the uniform deposition of Li⁺ ions and improve the Coulombic efficiency and energy density of batteries is a key task for the development of high-performance lithium metal anodes. Herein, a high-performance separator for lithium metal anodes was designed by the in situ growth of a metal–organic framework (MOF)-derived transition metal sulfide array as an artificial SEI on polypropylene separators (denoted as Co₉S₈-PP). The high ionic conductivity and excellent morphology provided a convenient transport path and fast charge transfer kinetics for lithium ions. The experimental data illustrate that, compared with commercial polypropylene separators, the Li//Cu half-cell with a Co₉S₈-PP separator can be cycled stably for 2000 h at 1 mA cm⁻² and 1 mAh cm⁻². Meanwhile, a Li//LiFePO₄ full cell with a Co₉S₈-PP separator exhibits ultra-long cycle stability at 0.2 C with an initial capacity of 148 mAh g⁻¹ and maintains 74% capacity after 1000 cycles. This work provides some new strategies for using transition metal sulfides to induce the uniform deposition of lithium ions to create high-performance lithium metal batteries. Full article

Graphite anode materials and carbonate electrolyte have been the top choices for commercial lithium-ion batteries (LIBS) for a long time. However, the uneven deposition and stripping of lithium cause irreversible damage to the graphite structure, and the low flash point and high flammability of the carbonate electrolyte pose a significant fire safety risk. Here, we proposed a multifunctional electrolyte additive diphenylphosphoryl azide (DPPA), which can construct a solid electrolyte interphase (SEI) with high ionic conductivity lithium nitride (Li₃N) to ensure efficient transport of Li⁺. This not only protects the artificial graphite (AG) electrode but also inhibits lithium dendrites to achieve excellent electrochemical performance. Meanwhile, the LIBS with DPPA offers satisfactory flame retardancy performance. The AG//Li half cells with DPPA-0.5M can still maintain a specific capacity of about 350 mAh/g after 200 cycles at 0.2 C. Its cycle performance and rate performance were better than commercial electrolyte (EC/DMC). After cycling, the microstructure surface of the AG electrode was complete and flat, and the surface of the lithium metal electrode had fewer lithium dendrites. Importantly, we found that the pouch cell with DPPA-0.5M had low peak heat release rate. When exposed to external conditions of continuous heating, DPPA significantly improved the fire safety of the LIBS. The research of DPPA in lithium electrolyte is a step towards the development of safe and efficient lithium batteries. Full article

The practical application of rechargeable aqueous zinc-ion batteries (ZIBs) has been severely hindered by detrimental dendrite growth, uncontrollable hydrogen evolution, and unfavorable side reactions occurring at the Zn metal anode. Here, we applied a Prussian blue analogue (PBA) material K₂Zn₃(Fe(CN)₆)₂ as an artificial solid electrolyte interphase (SEI), by which the plentiful -C≡N- ligands at the surface and the large channels in the open framework structure can operate as a highly zincophilic moderator and ion sieve, inducing fast and uniform nucleation and deposition of Zn. Additionally, the dense interface effectively prevents water molecules from approaching the Zn surface, thereby inhibiting the hydrogen-evolution-resultant side reactions and corrosion. The highly reversible Zn plating/stripping is evidenced by an elevated Coulombic efficiency of 99.87% over 600 cycles in a Zn/Cu cell and a prolonged lifetime of 860 h at 5 mA cm⁻², 2 mAh cm⁻² in a Zn/Zn symmetric cell. Furthermore, the PBA-coated Zn anode ensures the excellent rate and cycling performance of an α-MnO₂/Zn full cell. This work provides a simple and effective solution for the improvement of the Zn anode, advancing the commercialization of aqueous ZIBs. Full article