Batteries & Supercaps最新文献

The Front Cover illustrates the incorporation of potassium-containing poly(heptazine imide) (represented as triangles) into the pores of mesoporous carbon (hexagons). The resulting hybrid material exhibits higher electrical conductivity and a larger specific surface area than bulk ionic carbon nitride. This hybrid design enables the investigation of electric double-layer formation and interaction of K⁺ from the electrolyte at the PHI/electrolyte interface without the limiting effects of resistance. More information can be found in the Research Article by D. Leistenschneider and co-workers (DOI: 10.1002/batt.202500285).

Aqueous zinc-ion batteries (ZIBs) are a promising alternative to lithium-ion systems, offering intrinsic safety, environmental friendliness, and low cost. Among candidate cathode materials, manganese dioxide (MnO₂) stands out for its high theoretical capacity and abundance. However, translating MnO₂-based ZIBs from lab prototypes to practical devices remains challenging due to severe cycling stability issues. Key failure modes, including structural degradation of the MnO₂ cathode, manganese dissolution into the electrolyte with “dead” byproduct formation, sluggish Zn²⁺ diffusion and poor electronic conductivity, and unstable electrode/electrolyte interfaces, cause progressive capacity fade. These problems are further exacerbated under realistic operating conditions (thick electrodes, limited electrolyte, and prolonged cycling) required for commercial-level cells. This review provides a comprehensive analysis of these degradation mechanisms and critically surveys recent mitigation strategies such as MnO₂ nanostructuring and doping, protective surface coatings, and optimized aqueous electrolytes with additives. We also highlight the persistent performance gap between coin-cell demonstrations and real-world devices, emphasizing the need for in situ/operando diagnostic techniques, multiscale modeling, scalable electrode fabrication, and standardized testing protocols to better bridge that gap. By uniting fundamental insights with engineering solutions, this work offers guidelines to advance MnO₂-based ZIBs toward durable, high-performance energy storage devices suitable for broad application.

Understanding electrolyte degradation in electric double-layer capacitors (EDLCs) is essential for advancing high-temperature energy storage technologies. In this study, we present a comprehensive methodology to investigate temperature-induced electrolyte aging by correlating electrochemical behavior with molecular (bulk electrolyte) and interfacial (material surfaces) degradation processes. A custom-built Swagelok-type postmortem cell equipped with a quasi-reference silver wire enables simultaneous monitoring of the individual electrode potentials during operation and postaging access to both the liquid electrolyte and electrode surfaces. This integrated design allows for direct linkage between electrochemical response, liquid-phase degradation (via gas chromatography-mass spectrometry), and surface chemistry (via X-ray photoelectron spectroscopy). The methodology is validated across a matrix of electrolytes composed of the 1,1-dimethylpyrrolidinium tetrafluoroborate (Pyr₁₁BF₄) salt in either acetonitrile (ACN), the alternative solvent ethyl isopropyl sulfone (EiPS), and an ACN:EiPS 75:25, wt% mixture. All systems were subjected to accelerated aging through 24 h voltage float tests at 3.0 V and three temperatures (20°C, 40°C, and 65°C). By selecting PYR₁₁BF₄—known for its high electrochemical and thermal stability—the degradation pathways observed can be primarily attributed to solvent effects. This work highlights the critical link between solvent decomposition and electrochemical aging, demonstrating how multidimensional postmortem analysis can guide the development of high-voltage, temperature-stable EDLCs.

Carbon nanotubes (CNTs) have emerged as a promising conducting additive for next-generation high-capacity anode materials owing to their ability to form an electrically conductive network that maintains contact when subjected to significant volume expansion. However, as a result of their high porosity and surface area, CNTs currently suffer from poor initial irreversible capacity loss due to solid-electrolyte interphase (SEI) formation and excessive electrolyte consumption. Currently, there is limited understanding about how and where SEI forms on CNT-containing electrodes. In this work, electrochemical atomic force microscopy (EC-AFM) is employed to directly observe the influence of CNTs on SEI formation. By varying graphite:CNT ratio in casted electrodes, it is demonstrated that increasing CNT content results in earlier onset formation and a greater quantity of SEI. In addition, it is found that the SEI structure and nucleation behavior change with varying CNT concentration which has direct implications on the electrochemistry. Operando EC-AFM provides real-time visual insights into the SEI behavior which is critical for providing a more holistic understanding of the SEI formation. This work therefore helps redefine the role CNTs play within next-generation anode materials and the impact they have on SEI dynamics.

Currently, traditional recycling technologies for lithium-ion batteries (LIBs) are relatively mature, but their process pathways are difficult to adapt to the recycling needs of next-generation high-performance solid-state batteries (SSBs). As the global energy transition accelerates, SSBs are experiencing explosive growth due to their ultra-high energy density and inherent safety advantages. However, the large-scale industrialization of SSBs faces dual challenges: imbalances in the supply and demand of critical metal resources and heavy metal pollution from retired batteries. Compared with LIBs, SSBs have fundamental differences in material systems and the difficulty of solid–solid interface dissociation, and their recycling strategies are still in the early stages of exploration, with no closed-loop regeneration system yet established that is compatible with their material characteristics. This review systematically compares the fundamental differences between SSBs and LIBs in terms of recycling technology pathways, integrating innovative recycling and potential regeneration pathways for SSB cathode materials, various types of solid-state electrolytes (SSEs), and anode materials. It also outlines the future trends in SSB recycling technology toward multistrategy collaboration and standardized systems, laying the theoretical foundation for establishing an efficient, low-carbon, high-value industrial-scale recycling system for the comprehensive regeneration of all components of SSBs.

Nickel/zinc (Ni/Zn) batteries are a promising post-lithium technology for stationary energy storage applications offering advantages in safety, environmental compatibility, and resource availability. Although this battery chemistry has been known for decades, the theoretical knowledge about its electrochemical processes remains limited. In order to gain a deeper understanding of the general cycling behavior and the underlying processes, but also specific phenomena intrinsic to zinc-based cells such as zinc shape change, simulations based on a thermodynamically consistent, volume-averaged continuum model are performed. A Ni/Zn prototype cell is used as a reference framework to provide a basis for modeling, parameter estimation, and systematic comparison between simulated and experimental cell behavior to enhance cyclability and performance.

The lithium (Li) battery industry is constantly evolving, thanks to the introduction of novel materials, particularly anode materials, which contribute to the stability, capacity, and cyclability of the battery. This continuous development has led to the development of organic electrodes that are promising for their high capacity, tunable structure, and eco-friendly properties. However, challenges such as rapid capacity decay and poor cycle stability limit their practical usage. To provide solution for such issues, a novel multicarbonyl-based organic anode material, polyimide benzoquinone (PIBQ), which shows low solubility in conventional electrolytes and excellent Li storage performance, is reported. It delivers a high initial capacity of ≈823 mAh g⁻¹ and retains ≈530 mAh g⁻¹ after 450 cycles at 0.5C, with 64% capacity retention and nearly 100% coulombic efficiency (C.E.). In addition, the PIBQ cell shows an initial capacity of ≈645 mAh g⁻¹ at 1C displaying a unique self-stabilizing capacity behavior, increasing to ≈520 mAh g⁻¹ after 530 cycles and stable for 1000 cycles with capacity retention of ≈80% and ≈100% C.E. Experimental results show that the electrode exhibits a dominant pseudocapacitive charge storage behavior, especially within the testing potential window (93.5% at 1 mV s⁻¹), enabling fast charge kinetics. Density functional theory analysis shows that PIBQ's smaller highest occupied molecular orbital–lowest unoccupied molecular orbital gap contributes to enhance the energy storage capability.

To address interfacial challenges of the zinc anode in aqueous zinc-ion batteries (AZIBs), including dendrite growth and by-product formation, a carbon microspheres/carboxymethyl cellulose (CMC) composite coating (CCZn) is developed on the zinc foil. The composite coating achieves effective regulation of zinc deposition behavior through the synergistic effect of carbon microspheres and CMC. Specifically, the abundant oxygen-containing functional groups in the coating can form coordination bonds with the zinc substrate to enhance the mechanical stability of the anode. The CMC molecular chains fix the carbon microspheres through a hydrogen bond network to build a 3D stable framework, enabling rapid ion transport. Meanwhile, the rich carboxylate groups in the coating can promote the desolvation process of Zn(H₂O)₆²⁺, accelerating the kinetics of the zinc ion deposition process. In addition, the presence of the coating can cover the original surface defects of raw Zn (RZn), thereby uniformizing the electric field distribution on the electrode surface to inhibit dendrite growth. Consequently, the CCZn symmetric cell exhibits a cycle life 18 times longer than the RZn cell at 0.8 and 0.8 mAh cm⁻², highlighting its exceptional cycling durability. This work provides a novel interfacial engineering strategy to address zinc deposition challenges in AZIBs.

Aqueous ammonium-ion batteries (AAIBs) have gained considerable attention as a promising solution for sustainable energy storage owing to the natural abundance, cost-effectiveness, and biocompatibility of ammonium-ion (NH₄⁺) carriers, along with the intrinsic safety of aqueous electrolytes. Despite the considerable potential of manganese-based oxides for NH₄⁺ storage derived from their multiple valence states and diverse structures, existing research remains focused on Mn⁴⁺-based oxides, with low-valent manganese oxides largely unexplored. Herein, it is demonstrate that Mn₃O₄ nanoparticles can undergo in situ electrochemical reconstruction during cycling in aqueous (NH₄)₂SO₄ electrolyte, transforming into MnOOH (e-MnOOH) nanorods with an open channel structure and abundant defects. The resulting e-MnOOH exhibits significantly enhanced NH₄⁺ storage performance, providing a high specific capacity of 170.7 mAh g⁻¹ at 0.3 A g⁻¹, good rate capability. Besides, it also maintains 98.9% capacity retention after 300 cycles at 0.5 A g⁻¹. Ex situ characterizations reveal that the charge storage process is regulated by surface pseudocapacitance, which involves reversible Mn³⁺/Mn⁴⁺ redox and NH₄⁺ adsorption/desorption via hydrogen bonding. Furthermore, full AAIB is assembled by combining with an e-MnOOH cathode and PTCDA anode, which delivers a specific capacity of 91.7 mAh g⁻¹ and good cycling durability. This work not only unveils the electrochemical reconstruction behavior of low-valent Mn₃O₄ for NH₄⁺ storage but also provides insights into the pseudocapacitive NH₄⁺ storage in e-MnOOH beyond conventional MnO₂.

Tackling the dual challenges of global resource circularity and sustainable energy storage, this study pioneers a novel strategy for converting waste biomass (discarded cloth and paper) into high-performance composite anodes for sodium-ion batteries (SIBs) through a dual-engineering approach. Employing a gradient carbonization strategy, 3D porous carbon matrices retaining the intrinsic hierarchical architecture of the precursors are fabricated. Notably, the waste paper-derived carbon framework exhibits exceptional self-supporting properties. Subsequent vapor deposition enables the homogeneous encapsulation of red phosphorus (RP) throughout the carbon skeleton, yielding a stable Carbon@RP composite. Electrochemical evaluations demonstrate that the paper-derived Carbon@RP anode delivers a remarkable reversible capacity of 813.5 at 0.5 mA cm⁻². Mechanistic studies reveal that the paper-inherited “book-like” lamellar channel structure facilitates deep phosphorus infusion. This work establishes a closed-loop paradigm integrating “waste-to-energy storage” conversion, offering a practical and scalable pathway toward eco-friendly, high-energy-density SIBs for next-generation grid-scale renewable energy systems.