Remarkable Capacity Retention Research Articles

A Study on the Microstructure Regulation Effect of Niobium Doping on LiNi0.88Co0.05Mn0.07O2 and the Electrochemical Performance of the Composite Material under High Voltage.

High-nickel ternary materials are currently the most promising lithium battery cathode materials due to their development and application potential. Nevertheless, these materials encounter challenges like cation mixing, lattice oxygen loss, interfacial reactions, and microcracks. These issues are exacerbated at high voltages, compromising their cyclic stability and safety. In this study, we successfully prepared Nb5+-doped high-nickel ternary cathode materials via a high-temperature solid-phase method. We investigated the impact of Nb5+ doping on the microstructure and electrochemical properties of LiNi0.88Co0.05Mn0.07O2 ternary cathode materials by varying the amount of Nb2O5 added. The experimental results suggest that Nb5+ doping does not alter the crystal structure but modifies the particle morphology, yielding radially distributed, elongated, rod-like structures. This morphology effectively mitigates the anisotropic volume changes during cycling, thereby bolstering the material's cyclic stability. The material exhibits a discharge capacity of 224.4 mAh g-1 at 0.1C and 200.3 mAh g-1 at 1C, within a voltage range of 2.7 V-4.5 V. Following 100 cycles at 1C, the capacity retention rate maintains a high level of 92.9%, highlighting the material's remarkable capacity retention and cyclic stability under high-voltage conditions. The enhancement of cyclic stability is primarily due to the synergistic effects caused by Nb5+ doping. Nb5+ modifies the particle morphology, thereby mitigating the formation of microcracks. The formation of high-energy Nb-O bonds prevents oxygen precipitation at high voltages, minimizes the irreversibility of the H2-H3 phase transition, and thereby enhances the stability of the composite material at high voltages.

Unleashing the impact of Nb-doped, single crystal, cobalt-free P2-type Na0.67Ni0.33Mn0.67O2 on elevating the cycle life of sodium-ion batteries

A synergistic stabilization effect in a Nb-doped P2-type single crystal cobalt-free layered oxide cathode material, offering remarkable cycling stability and high-power performance for Na-ion batteries have unveiled in this study. The introduction of Nb in the transition metal layer not only reduces the electronic band gap but also enhances electronic conductivity and mitigates ionic diffusion energy barriers. The induction of a robust Nb-O bond expedites electron and Na+ transfer, contributing to the stabilization of the host structure is further confirmed through the density functional theory calculations, including electron localization function (ELF) and crystal orbital Hamiltonian population (COHP). To the best of our knowledge, this study is the first to demonstrate a homogeneous distribution of niobium throughout the single crystal, specifically doped at the nickel site within the bulk, without inducing atomic-scale surface reorganization. The presence of single crystals improves various kinetic factors, demonstrating the profound correlation between structural defects and chemical proliferation, thereby reducing the evolution of oxygen gas. The P2-type Nb-doped single crystal cathode (Na0.67Ni0.31Mn0.67Nb0.02O2) exhibits remarkable capacity retention, >95 % after 100 cycles at 0.1 C and >90 % after an extended cycling of 2000 cycles at 1 C. Practical assessments in complete cell setups with a pre-sodiated hard carbon anode further validate the material's viability, showcasing capacity retention of over 93 % after 100 cycles in a coin cell and approximately 89 % in a pouch cell format. This comprehensive study establishes the transformative potential of Nb-doped single crystal cobalt-free P2-type layered oxide cathode materials, marking a significant advancement in sodium-ion battery technology.

Continuous Flow Electrochemical Synthesis of Olivine-Structured NaFePO4 Cathode Material for Sodium-Ion Batteries from Recycle LiFePO4.

To mitigate the environmental impact of the improper disposal of spent LiFePO4 batteries and reduce resource waste, the development of LiFePO4 recycling technologies is of paramount importance. Meanwhile, olivine-structured NaFePO4 in sodium-ion batteries has received great attention, due to its high theoretical specific capacity of 154 mAh g-1 and excellent stability. However, olivine NaFePO4 only can be synthesized from olivine LiFePO4. Accordingly, in this proposal, developing the continuous flow electrochemical solid-liquid reactor-based metal ion insertion technology is to utilize the olivine FePO4, recycled from LiFePO4, and to synthesize NaFePO4. Additionally, by employing I- as the reducing agent, NaFePO4 is successfully synthesized with a discharge-specific capacity of 134 mAh g-1 at 0.1C and a remarkable capacity retention rate of 86.5% after 100 cycles at 0.2C. And the reasons for sodium deficiency in the synthesized NFP are elucidated through first-principles calculations. Furthermore, the kinetics of the solid-solution reaction 2 (Na2/3+βPO4→ Na1-αFePO4) mechanism improve with cycling and are sensitive to temperature. Utilizing a minimal amount of reducing agent in the electrochemical reactor, NaFePO4 synthesis is successfully achieved. This innovative approach offers a new, cost-effective, and environmentally friendly strategy for preparing NaFePO4 from recycling LiFePO4.

Ultrathin, Mechanically Robust Quasi-Solid Composite Electrolyte for Solid-State Lithium Metal Batteries.

Herein, we present the preparation and properties of an ultrathin, mechanically robust, quasi-solid composite electrolyte (SEO-QSCE) for solid-state lithium metal battery (SLB) from a well-defined polystyrene-b-poly(ethylene oxide) diblock copolymer (SEO), Li6.75La3Zr1.75Ta0.25O12 nanofiller, and fluoroethylene carbonate plasticizer. Compared with the ordered lamellar microphase separation of SEO, the SEO-QSCE displays bicontinuous phases, consisting of a Li+ ion conductive poly(ethylene oxide) domain and a mechanically robust framework of the polystyrene domain. Therefore, the 12 μm-thick SEO-QSCE membrane exhibits an exceptional ionic conductivity of 1.3 × 10-3 S cm-1 at 30 °C, along with a remarkable tensile strength of 5.1 MPa and an elastic modulus of 2.7 GPa. The high mechanical robustness and the self-generated LiF-rich SEI enable the SEO-QSCE to have an extraordinary lithium dendrite prohibition effect. The SLB of Li|SEO-QSCE|LiFePO4 reveals superior cycling performances at 30 °C for over 600 cycles, maintaining an initial discharge capacity of 145 mAh g-1 and a remarkable capacity retention of 81% (117 mAh g-1) after 400 cycles at 0.5 C. The high-voltage SLB of Li|SEO-QSCE|LiNi0.5Co0.3Mn0.2O2 displays good cycling stability for over 150 cycles at 30 °C. Moreover, the exceptional robustness of SEO-QSCE enables the high-voltage solid-state pouch cell of Li|SEO-QSCE|LiNi0.5Co0.3Mn0.2O2 with high flexibility and excellent safety features. The current investigation delivers a promising and innovative approach for preparing quasi-solid electrolytes with features of ultrathin design, mechanical robustness, and exceptional electrochemical performance for high-voltage SLBs.

Inhibition of Vanadium Cathode Dissolution in Zinc‐Ion Batteries on Thermodynamics and Kinetics by Guest Pre‐Intercalation

AbstractAqueous zinc‐ion batteries (AZIBs), recognized for their safety and environmental friendliness, hold significant promise for large‐scale energy storage. However, the rapid capacity degradation resulting from the dissolution of active cathode materials hampers the advancement of AZIBs. Here, Ru0.2V2O5∙0.41H2O (RuVO) is synthesized with remarkable capacity retention (98.2% over 5000 cycles at 10 A g−1). The pre‐intercalation of Ru3+ enhances the stability of both intrinsic and cycling structures, elevating the Gibbs free energy and suppressing V‐dissolution thermodynamically. Additionally, Ru3+ intercalation modulates the potential energy surface of Zn2+ migration, leading to the dominance of Zn2+ in the insertion/extraction mechanism, thereby kinetically impeding the dissolution reaction. This study elucidates the dissolution thermodynamics and kinetics of V‐based cathodes through a combination of experiments, mechanism analyses, and density functional theory (DFT) calculations.

In Situ Formation of Heterojunction in Composite Lithium Anode Facilitates Fast and Uniform Interfacial Ion Transport.

Lithium metal is a highly promising anode for next-generation high-energy-density rechargeable batteries. Nevertheless, its practical application faces challenges due to the uncontrolled lithium dendrites growth and infinite volumetric expansion during repetitive cycling. Herein, a composite lithium anode is designed by mechanically rolling and pressing a cerium oxide-coated carbon textile with lithium foil (Li@CeO2/CT). The in situ generated cerium dioxide (CeO2) and cerium trioxide (Ce2O3) form a heterojunction with a reduced lithium-ion migration barrier, facilitating the rapid lithium ions migration. Additionally, both CeO2 and Ce2O3 exhibit higher adsorbed energy with lithium, enabling faster and more distributed interfacial transport of lithium ions. Furthermore, the high specific surface area of 3D skeleton can effectively reduce local current density, and alleviate the lithium volumetric changes upon plating/stripping. Benefiting from this unique structure, the highly compact and uniform lithium deposition is constructed, allowing the Li@CeO2/CT symmetric cells to maintain a stable cycling for over 500 cycles at an exceptional high current density of 100 mA cm-2. When paired with LiNi0.91Co0.06Mn0.03O2 (NCM91) cathode, the cell achieves 74.3% capacity retention after 800 cycles at 1 C, and a remarkable capacity retention of 81.1% after 500 cycles even at a high rate of 4C.

Revealing the effect of cobalt content and ligand exchange in the bimetallic Ni–Co MOF for stable supercapacitors with high energy density

Metal-organic frameworks (MOF) exhibit considerable potential as electrode materials for supercapacitors. Nevertheless, the electrochemical performance of the MOF is impeded by its low electrical conductivity and chemical stability. In this study, we investigate the impact of cobalt composition and ligand exchange on the performance of bimetallic NiCo-MOF to unlock its optimal performance. Our results reveal that integrating cobalt affects the abundance of Ni3+ and Co2+, which serve as electrochemical active species. Additionally, ligand exchange with a phosphate group leads to further modifications in both abundance and surface area. The result indicates that a Ni/Co ratio of 10:1 in NiCo-MOF exhibits superior performance (437 C g−1 at 0.5 A g−1), surpassing the performance of other ratios. Furthermore, the process of ligand exchange in NiCo-MOF with a Ni/Co ratio of 10:1 yields an even higher capacity of 522 C g−1 at 0.5 A g−1, with an energy density of 22 Wh kg−1 at 363 W kg−1 when assembled in an asymmetric supercapacitor cell. The supercapacitor cell demonstrates a remarkable capacity retention of 99 % at 5 A g−1 over 5000 cycles. This study provides insight into the pivotal role of cobalt composition and ligand exchange in improving the electrochemical performance of NiCo-MOF.

Mechanistic Study on Artificial Stabilization of Lithium Metal Anode via Thermal Pyrolysis of Ammonium Fluoride in Lithium Metal Batteries.

The use of the "Holy Grail" lithium metal anode is pivotal to achieve superior energy density. However, the practice of a lithium metal anode faces practical challenges due to the thermodynamic instability of lithium metal and dendrite growth. Herein, an artificial stabilization of lithium metal was carried out via the thermal pyrolysis of the NH4F salt, which generates HF(g) and NH3(g). An exposure of lithium metal to the generated gas induces a spontaneous reaction that forms multiple solid electrolyte interface (SEI) components, such as LiF, Li3N, Li2NH, LiNH2, and LiH, from a single salt. The artificially multilayered protection on lithium metal (AF-Li) sustains stable lithium stripping/plating. It suppresses the Li dendrite under the Li||Li symmetric cell. The half-cell Li||Cu and Li||MCMB systems depicted the attributions of the protective layer. We demonstrate that the desirable protective layer in AF-Li exhibited remarkable capacity retention (CR) results. LiFePO4 (LFP) showed a CR of 90.6% at 0.5 mA cm-2 after 280 cycles, and LiNi0.5Mn0.3Co0.2O2 (NCM523) showed 58.7% at 3 mA cm-2 after 410 cycles. Formulating the multilayered protection, with the simultaneous formation of multiple SEI components in a facile and cost-effective approach from NH4F as a single salt, made the system competent.

Reconstruction of solvation structure at the cathode-electrolyte interface via partial de-solvation in a metal-organic framework

The formation of cathode-electrolyte interphase (CEI) is closely related to the solvation structure in direct contact with the cathode. The de-solvated solvent molecules are subject to the attack of highly catalytic transition metal ions in the cathode materials (such as Ni-rich LiNi0.8Co0.1Mn0.1O2, Ni-rich NCM), especially at high voltage or high temperature, leading to the poor CEI structure that accelerates the deterioration of rechargeable batteries. Considerable strategies have been proposed to solve this issue. Herein, we have constructed a porous Mg-MOF buffer layer on the surface of Ni-rich NCM, which not only greatly reduces the contact between solvent molecules and cathodes to alleviate the extensive interface reactions, but also promote the de-solvation of Li+ solvation structure through strong affinity between solvents and Mg2+. The partially de-solvated structure induces the anion to participate in the solvation structure and contributes to the formation of a uniform LiF-rich CEI with superior mechanical integrity and chemical stability. Therefore, the NCM with Mg-MOF buffer layer exhibits improved cycling stability at both elevated temperature of 45 °C and high voltage of 4.5 V with lithium as anode. Moreover, the modified NCM/graphite full cells also deliver ultra-stable rechargeable capability with a remarkable capacity retention of 87.3% over 1000 cycles as compared to the only 21.7% of pristine NCM based cells.

Design of high-entropy P2/O3 hybrid layered oxide cathode material for high-capacity and high-rate sodium-ion batteries

High-entropy layered cathode materials have garnered significant attention due to their exceptional structural stability and capacity retention. However, the complex composition of these materials has posed challenges for performance optimization. Herein, an innovative high-entropy P2/O3 hybrid layered oxide cathode material with impressive reversible capacity and high-rate capabilities is designed according to the configurational entropy adjustment strategy. Specifically, the unique structure of Na0.85Li0.05Ni0.3Fe0.1Mn0.5Ti0.05O2 (LNFMT) exhibits not only enhanced anionic activity but also mitigated migration of transition metals at high voltage. The high-entropy effect facilitates the migration of Li+ to Na layer, forming a pseudo-tetrahedral structure that hinders the movement of Fe3+. Additionally, the robust Ti-O bond ensures the internal cohesion of transition metal layers, enhancing the structural stability during de-/intercalation processes. As a result, the undesirable P2-O2 phase transformation is effectively suppressed in 1.5–4.5 V, leading to a remarkable capacity retention of over 70% after 100 cycles at 0.2 C. Moreover, LNFMT shows a high discharge capacity of 116 mAh/g at 10 C with excellent capacity retention of 94.23% after 150 cycles in 2.0–4.2 V, demonstrating its superior rate capability. This research showcases the significant impact of the high-entropy effect and provides a novel perspective for the design of sodium-ion cathode materials.

Designer Lithium Reservoirs for Ultralong Life Lithium Batteries for Grid Storage.

The minimization of irreversible active lithium loss stands as a pivotal concern in rechargeable lithium batteries, particularly in the context of grid-storage applications, where achieving the utmost energy density over prolonged cycling is imperative to meet stringent demands, notably in terms of life cost. Departing from conventional methodologies advocating electrode prelithiation and/or electrolyte additives, a new paradigm is proposed here: the integration of a designer lithium reservoir (DLR) featuring lithium orthosilicate (Li4SiO4) and elemental sulfur. This approach concurrently addresses active lithium consumption through solid electrolyte interphase (SEI) formation and mitigates minor yet continuous parasitic reactions at the electrode/electrolyte interface during extended cycling. The remarkable synergy between the Li-ion conductive Li4SiO4 and the SEI-favorable elemental sulfur enables customizable compensation kinetics for active lithium loss throughout continuous cycling. The introduction of a minute quantity of DLR (3 wt% Li4SiO4@S) yields outstanding cycling stability in a prototype pouch cell (graphite||LiFePO4) with an ampere-hour-level capacity (≈2.3 Ah), demonstrating remarkable capacity retention (≈95%) even after 3000 cycles. This utilization of a DLR is poised to expedite the development of enduring lithium batteries for grid-storage applications and stimulate the design of practical, implantable rechargeable batteries based on related cell chemistries.

Self-adhesive, freeze-tolerant, and strong hydrogel electrolyte containing xanthan gum enables the high-performance of zinc-ion hybrid supercapacitors

Hydrogel electrolyte is an ideal candidate material for flexible energy storage devices due to its excellent softness and conductivity properties. However, challenges such as the inherent mechanical weakness, the susceptibility to be frozen in low-temperature environments, and the insufficiency of hydrogel-electrode contact persist. Herein, a “Multi in One” strategy is employed to effectively conquer these difficulties by endowing hydrogels with high strength, freeze-resistance, and self-adhesive ability. Multiple hydrogen bond networks and ion crosslinking networks are constructed within the hydrogel electrolyte (PVA/PAAc/XG) containing polyvinyl alcohol (PVA), acrylic acid (AAc), and xanthan gum (XG), promoting the enhanced mechanical property, and the adhesion to electrode materials is also improved through abundant active groups. The introduction of zinc ions provides the material with superior frost resistance while also promoting electrical conductivity. Leveraging its multifunction of superior mechanical strength, anti-freeze property, and self-adhesive characteristic, the PVA/PAAc/XG hydrogel electrolyte is employed to fabricate zinc ion hybrid supercapacitors (ZHS). Remarkably, ZHS exhibits outstanding electrochemical performance and cycle stability. A remarkable capacity retention rate of 83.86 % after 10,000 charge-discharge cycles can be achieved at high current densities, even when the operational temperature decreases to −60 °C, showing great potential in the field of flexible energy storage devices.

Tuning surface chemistry to reduce the step-like degradation of LiCoO2 at 4.6 V

Elevating the cut-off voltage is an effective route to increase the energy density of LiCoO2 (LCO). However, the highly delithiated LCO faces the issues of poor structural reversibility, O loss, and Co dissolution, etc., especially in the surface region. Herein, the step-like surface degradation (SSD) of pristine LCO (P-LCO) is firstly revealed to be responsible for the rapid capacity decay. To reduce the adverse impact of SSD, a solid electrolyte is coated and annealed to achieve the optimized surface structure chemistry of LCO (SE-LCO), featuring the outermost surface Li3PO4, surface rock-salt layer, and subsurface spinel-like layer. Benefiting from this surface optimization, the SE-LCO not only shows an enhanced but more reversible phase transition to enhance the structure stability, but also promotes the formation of tough cathode electrolyte interface (CEI) to reduce the O loss and Co dissolution issues. As a result, SE-LCO/graphite cell achieves excellent cycle stability with a remarkable capacity retention of 81.2% after 800 cycles in a potential range of 3–4.55 V, which is among the best reported cell performances. This work broadens the cognition for developing more advanced LCO cathodes.

Confluence of ZnO and PTFE Binder for Enhancing Performance of Thin‐Film Lithium‐Ion Batteries

Developing anode materials with high specific capacity and cycling stability is vital for improving thin‐film lithium‐ion batteries. Thin‐film zinc oxide (ZnO) holds promise due to its high specific capacity, but it suffers from volume changes and structural stress during cycling, leading to poor battery performance. In this research, we ingeniously combined polytetrafluoroethylene (PTFE) with ZnO using a radio frequency (RF) magnetron co‐sputtering method, ensuring a strong bond in the thin‐film composite electrode. PTFE effectively reduced stress on the active material and mitigated volume change effects during Li+ ion intercalation and deintercalation. The composite thin films are thoroughly characterized using advanced techniques such as X‐ray diffraction, scanning electron microscopy, and X‐ray photoelectron spectroscopy for investigating correlations between material properties and electrochemical behaviors. Notably, the ZnO/PTFE thin‐film electrode demonstrated an impressive specific capacity of 1305 mAh g−1 (=7116 mAh cm−3) at a 0.5C rate and a remarkable capacity retention of 82% from the 1st to the 100th cycle, surpassing the bare ZnO thin film (50%). This study provides valuable insights into using binders to stabilize active materials in thin‐film batteries, enhancing battery performance.

One‐Step Preparation Pitch‐Based Porous Carbon via Carbonization and Co‐Activation for High‐Performance Supercapacitors

AbstractHierarchical porous carbon (HPC) materials for supercapacitor (SC) application are synthesized via a one‐step carbonization and activation method, using a novel composite activating agent with synergistic activation effect from mesophase pitch (MP) as precursor. The prepared mesophase pitch‐based porous carbon (MPPC) exhibits an ultra‐high specific surface area (SSA) of 2955.0 m2 g−1, well‐controlled pore size distribution (PSD), and exceptional electrochemical performance. The specific capacitance of MPPC‐4 attains up to 338.1 F g−1 at 1 A g−1 and 250.1 F g−1 at 20 A g−1, demonstrating remarkable rate capability. Furthermore, the assembled symmetric SC achieves a high energy density of 29.83 Wh kg−1 at a power density of 999.93 W kg−1 and still maintains 6.56 Wh kg−1 at a high power density of 19.89 kW kg−1. Furthermore, the SC exhibits advantageous cyclic stability, as evidenced by its remarkable capacitance retention rate of 88.55 % even after 5000 cycles. The utilization of this novel composite activating agent in the synthesis of pitch‐derived porous carbon (PC) electrode materials is an exceptionally effective and inventive process.

Tuning the Interface Stability of Nickel-Rich NCM Cathode Against Aggressive Structural Collapse via the Synergistic Effect of Additives.

Nickel-rich layered oxides are envisaged as one of the most promising alternative cathode materials for lithium-ion batteries, considering their capabilities to achieve ultrahigh energy density at an affordable cost. Nonetheless, with increasing Ni content in the cathodes comes a severe extent of Ni4+ redox side reactions on the interface, leading to fast capacity decay and structural stability fading over extended cycles. Herein, dual additives of bis(vinylsulfonyl)methane (BVM) and lithium difluorophosphate (LiDFP) are adopted to synergistically generate the F-, P-, and S-rich passivation layer on the cathode, and the Ni4+ activity and dissolution at high voltage are restricted. The sulfur-rich layer formed by the polymerization of BVM, combined with the Li3PO4 and LiF phases derived from LiDFP, alleviates the problems of increased impedance, cracks, and an irreversible H2-H3 phase transition. Consequently, the Ni-rich LiNixM1-xO2 (x > 0.95) button half-cell cycled in LiDFP + BVM electrolyte exhibits a significant discharging capacity of 181.4 mAh g-1 at 1 C (1 C = 200 mA g-1) with retention of 83.7% after 100 cycles, surpassing the performance of the commercial electrolyte (160.7 mAh g-1) with retention of 53.3%. Remarkably, the NCM95||graphite pouch cell exhibits a remarkable capacity retention of 95.5% after 200 cycles. This work inspires the rational design of electrolyte additives for ultrahigh-energy batteries with nickel-rich layered oxide cathodes.

Constructing high-toughness polyimide binder with robust polarity and ion-conductive mechanisms ensuring long-term operational stability of silicon-based anodes

Silicon-based materials have demonstrated remarkable potential in high-energy–density batteries owing to their high theoretical capacity. However, the significant volume expansion of silicon seriously hinders its utilization as a lithium-ion anode. Herein, a functionalized high-toughness polyimide (PDMI) is synthesized by copolymerizing the 4,4′-Oxydiphthalic anhydride (ODPA) with 4,4′-oxydianiline (ODA), 2,3-diaminobenzoic acid (DABA), and 1,3-bis(3-aminopropyl)-tetramethyl disiloxane (DMS). The combination of rigid benzene rings and flexible oxygen groups (-O-) in the PDMI molecular chain via a rigidness/softness coupling mechanism contributes to high toughness. The plentiful polar carboxyl (–COOH) groups establish robust bonding strength. Rapid ionic transport is achieved by incorporating the flexible siloxane segment (Si-O-Si), which imparts high molecular chain motility and augments free volume holes to facilitate lithium-ion transport (9.8 × 10−10 cm2 s−1 vs. 16 × 10−10 cm2 s−1). As expected, the SiOx@PDMI-1.5 electrode delivers brilliant long-term cycle performance with a remarkable capacity retention of 85% over 500 cycles at 1.3 A g−1. The well-designed functionalized polyimide also significantly enhances the electrochemical properties of Si nanoparticles electrode. Meanwhile, the assembled SiOx@PDMI-1.5/NCM811 full cell delivers a high retention of 80% after 100 cycles. The perspective of the binder design strategy based on polyimide modification delivers a novel path toward high-capacity electrodes for high-energy–density batteries.

High-Fluidity/High-Strength Dual-Layer Gel Electrolytes Enable Ultra-Flexible and Dendrite-Free Fiber-Shaped Aqueous Zinc Metal Battery.

Fiber-shaped aqueous zinc-ion batteries (FAZIBs) with intrinsic safety, highcapacity, and superb omnidirectional flexibility hold promise for wearable energy-supply devices. However, the interfacial separation of fiber-shaped electrodes and electrolytes caused by Zinc (Zn) stripping process and severe Zn dendrites occurring at the folded area under bending condition seriously restricts FAZIBs' practical application. Here, an advanced confinement encapsulation strategy is originally reported to construct dual-layer gel electrolyte consisting of high-fluidity polyvinyl alcohol-Zn acetate inner layer and high-strength Zn alginate outer layer for fiber-shaped Zn anode. Benefiting from the synergistic effect of inner-outer gel electrolyte and the formation of solid electrolyte interphaseon Zn anode surface by lysine additive, the resulting fiber-shaped Zn-Zn symmetric cell delivers long cycling life over 800h at 1 mA cm-2 with dynamic bending frequency of 0.1Hz. The finite element simulation further confirms that dual-layer gel electrolyte can effectively suppress the interfacial separation arising from the Zn stripping and bending process. More importantly, a robust twisted fiber-shaped Zn/zinc hexacyanoferrate battery based on dual-layer gel electrolyte is successfully assembled, achieving a remarkable capacity retention of 97.7% after bending 500 cycles. Therefore, such novel dual-layer gel electrolyte design paves the way for the development of long-life fiber-shaped aqueous metal batteries.

Nanoarchitectonics of self-supporting porous carbon electrode with heteroatoms co-doped: For high-performance supercapacitors

Wood possesses a uniform hierarchical porous structure and high mechanical strength, rendering it an excellent precursor for the preparation of self-supporting carbon electrodes without binders and conductive agents. This paper presents an efficient method for synthesizing a self-supporting carbon electrode (HCW-0.7) with high specific surface area, hierarchical pore structure and abundant surface functional groups, utilizing simple hydrothermal pre-treatment and one-step thermochemical conversion process. The HCW-0.7 electrode demonstrates remarkable electrochemical performance, achieving an excellent specific capacitance of 298.52 F g−1 under a current density of 0.5 A g−1. The wood-based symmetrical supercapacitor (HSC) constructed with HCW-0.7 as the electrode has excellent energy density, power density and rate performance. At the power density of 287.5 W kg−1, HSC demonstrates an energy density of 9.43 Wh kg−1, exhibits its excellent electrochemical performance. Notably, even when subject to a higher power density of 5750 W kg−1, the energy density remains at 5.16 Wh kg−1. Furthermore, even after 20,000 charge and discharge cycles, HSC demonstrates a remarkable capacity retention rate of 96.24 %.

Evolving non-aggregated ZIF-8 nanoparticles into hierarchically porous hollow carbon nanofibers for high-performance flexible zinc-ion hybrid supercapacitor

Zinc-ion hybrid supercapacitors are garnering widespread interest in wearable energy storage devices due to their high power density, intrinsic safety and cost-effectiveness. However, the primary obstacle to their progress lies in the scarcity of cathode materials that concurrently demonstrate excellent flexibility and high energy density. Herein, we deliberately design a coaxial electrospinning ZIF-8 derived hollow carbon nanofiber film electrode (C-PAN(ZIF-8)@PVP) to achieve high-performance flexible ZHSCs. The distinctive configuration of C-PAN(ZIF-8)@PVP electrode comprises a shell of homogeneously distributed ZIF-8 derived porous carbon nanoparticles, which are bound together by N-doped carbon fibers derived from polyacrylonitrile (PAN), and a channel through the fiber created by the decomposition of polyvinylpyrrolidone (PVP). This unique architecture coupled with N, O co-doping bestows ample electrolyte infiltration, complete exposure of active sites, and a rapid pathway for electron conduction, resulting in facilitated ion diffusion kinetics, abundant active sites and enhanced electronic conductivity of the C-PAN(ZIF-8)@PVP electrode. As a result, the assembled ZHSC delivers a high reversible capacity of 116 mAh g−1 at 0.1 A g−1 and remarkable capacity retention of 100% over 4000 cycles at 5 A g−1. Moreover, it exhibits exceptional mechanical flexibility, capable of delivering stable output under arbitrary deformation. The intricate structural design strategy offers valuable insights for the development of high-performance electrode materials.