Ion Transport Pathways Research Articles

In-Situ Preparation of Iron(II)-phthalocyanine@multi-Walled-CNTs Nanocomposite for Quasi-Solid-State Flexible Symmetric Supercapacitors with Long Cycling Life.

The construction of supercapacitor electrode materials with exceptional performance is crucial to the commercialisation of flexible supercapacitors. Here, a novel in-situ precipitation technique was applied for constructing iron(II)-phthalocyanine (FePc) based nanocomposite as the electrode material in quasi-solid-state flexible supercapacitors. The highly redox-active FePc nanostructures were grown in the multi-walled-CNTs (MWCNTs) networks, which shows convenient electron/electrolyte ion transport pathways along with outstanding structural stability, leading to high energy storage and long cycling life. The electrode of FePc@MWCNTs delivered a higher specific capacity than that of individual MWCNTs and FePc. The quasi-solid-state symmetric flexible device that was constructed using FePc@MWCNTs electrode demonstrated impressive performance with a maximum energy density of 29.7 Wh kg-1 and a maximum power density of 4000 W kg-1. Moreover, the device demonstrated superior durability and flexibility, as evidenced by its exceptional cyclic stability (111.3 %) even after 30000 cycles at 8 A g-1. These results reveal that the FePc@MWCNTs nanocomposite prepared by this simple in-situ precipitation method is promising as electrode material for next-generation flexible wearable power sources.

High-Performance Solid-State Lithium Metal Batteries of Garnet/Polymer Composite Thin-Film Electrolyte with Domain-Limited Ion Transport Pathways.

The integrated approach of interfacial engineering and composite electrolytes is crucial for the market application of Li metal batteries (LMBs). A 22 μm thin-film type polymer/Li6.4La3Zr1.4Ta0.6O12 (LLZTO) composite solid-state electrolyte (LPCE) was designed that combines fast ion conduction and stable interfacial evolution, enhancing lithium metal interface stability and cycling performance. The ether-based molecular coordination groups/clusters formed by triethylene glycol dimethyl ether (TGDE) and anions facilitated the movement of Li+ between the polymer chain segments. These specific coordination clusters significantly "constrained" the interaction between anions and Li+, inducing the anions to follow the clusters to the Li metal and preferentially participate in solid electrolyte interface (SEI) derivatization. The inorganic salt-rich gradient SEI modulates Li+ deposition and inhibits uncontrolled dendrite growth, achieving stable cycling of Li symmetric cell at 0.2 mA cm-2 for over 2000 h. Furthermore, the Li||NCM811 cell at a rate of 0.1 C exhibits an initial discharge capacity of 194.5 mAh g-1, maintaining a capacity retention rate of over 90% after 500 cycles. This work demonstrates the importance of domain-limited ion clusters in ion transport and interfacial evolution, providing a perspective for solid-state LMBs.

Enabling High‐Rate and Long‐Cycling Zinc–Air Batteries with a ΔE = 0.56 V Bifunctional Oxygen Electrocatalyst

AbstractZn–air batteries (ZABs) are promising next‐generation energy storage devices due to their low cost, intrinsic safety, and environmental benignity. However, the sluggish kinetics of the cathodic reactions severely limits the ZAB performances in practical use, calling for high‐efficiency bifunctional oxygen reduction and evolution electrocatalysts. Herein, an ultrahigh‐active bifunctional electrocatalyst is developed with a record‐low ΔE of 0.56 V, significantly outperforming the noble‐metal‐based benchmark (Pt/C+Ir/C, ΔE = 0.77 V) and many other reported bifunctional electrocatalysts (mostly ΔE ≥ 0.60 V). The nanoscale composite of Fe‐based single‐atom sites and nanosized layered double hydroxides endows the bifunctional electrocatalyst with high conductivity and a large active surface that afford strengthened electron conduction and ion transport pathways. Furthermore, a remarkable improvement in stability is realized following the current division principle. ZABs with the bifunctional electrocatalyst deliver a high peak power density of 198 mW cm−2 and excellent cycling durability for over 6000 cycles. Moreover, ampere‐hour‐scale ZABs are constructed and cycled under 1.0 A and 1.0 Ah conditions. This work breaks the activity record for bifunctional oxygen electrocatalysis and expands the potential of ZABs for sustainable energy storage.

Wood‐inspired High Ionic Conductivity Hydrogel Electrolytes for Flexible Supercapacitors

Hydrogel is a promising electrolyte substrate, but its ionic conductivity needs further improvement. In this paper, we propose a strategy to improve the ionic conductivity of hydrogels with flexible wood and fabricate a flexible wood‐based poly(acrylic acid‐acrylamide) composite hydrogel electrolyte (WHE) by delignification and in‐situ polymerization. The flexible wood as a porous backbone for hydrogels can regulate ion transport pathways to improve the ionic conductivity of hydrogels. The straight pores of wood confine the transport of electrolyte ions along the shortest path, resulting in a high ionic conductivity of 3.0 × 10‐2 S cm‐1, which is great in composite polymer electrolytes. We have systematically investigated the effect of the degree of delignification and the polymerization process on the overall performance of the electrolyte. The optimized supercapacitor exhibits a specific capacitance of 155.64 F g‐1 and an energy density of 7.45 W h kg‐1. The WHE is applied to flexible supercapacitor, which exhibits good flexibility under bending conditions and can maintain similar electrochemical performance at a wide range of bending angles. This work provides an effective strategy for the efficient use of wood resources and the development of low‐cost, environmentally friendly, and high‐performance hydrogel electrolyte materials.

3D-printed Bio-inspired porous electrode by bidirectional enhancement strategy with high mass loading and enhanced energy density for supercapacitors

The effective strategy for increasing areal capacity involves the use of 3D printed thick-electrode with high mass loading. However, thick-electrode still encounters challenges such as incomplete electrolyte penetration and slow ion transport. Here, we successfully prepared lignocellulosic nanofibrils (LCNFs) from abundant bamboo biomass and developed functional ink composed of LCNFs/ carbon nanotubes (CNTs) / polyaniline (PANI) / polyvinyl alcohol (PVA) for printing. An innovative 3D printing bidirectional enhancement strategy was proposed to increase the mass loading of active materials in the vertical direction and construct ion transport channels in the transverse direction. The biomimetic porous N-doped electrode obtained after annealing treatment exhibits a more continuous conductive network, larger surface area, higher utilization of active materials, and smoother ion transport pathways compared to thick-electrode. Therefore, the Triangles biomimetic electrode exhibits an enhanced areal/specific capacitance compared to thick-electrode, reaching 5.30F·cm−2 (184.03F·g−1) and 4.40F·cm−2 (122.22F·g−1) at 2 mA·cm−2, respectively. The symmetric device demonstrates an areal capacitance of 1.34F·cm−2 at 1 mA·cm−2 and achieves an energy density of 0.186 mWh·cm−2 at a power density of 0.49 mW·cm−2. The work provides valuable insights into the design of electrode structures for high-performance supercapacitors.

Designing Cooperative Ion Transport Pathway in Ultra‐Thin Solid‐State Electrolytes toward Practical Lithium Metal Batteries

AbstractSolid polymer electrolytes (SPEs) are promising for high‐energy‐density solid‐state Li metal batteries due to their decent flexibility, safety, and interfacial stability. However, their development was seriously hindered by the interfacial instability and limited conductivity, leading to inferior electrochemical performance. Herein, we proposed to design ultra‐thin solid‐state electrolyte with long‐range cooperative ion transport pathway to effectively increase the ionic conductivity and stability. The impregnation of PVDF−HFP inside pores of fluorinated covalent organic framework (CF3−COF) can disrupt its symmetry, rendering rapid ion transportation and inhibited anion immigration. The functional groups of CF3−COF can interact with PVDF−HFP to form fast Li+ transport channels, which enables the uniform and confined Li+ conduction within the electrolyte. The introduction of CF3−COF also enhances the mechanical strength and flexibility of SPEs, as well as ensures homogeneous Li deposition and inhibited dendrite growth. Hence, a remarkably high conductivity of 1.21×10−3 S cm−1 can be achieved. Finally, the ultra‐thin SPEs with an extremely long cycle life exceed 9000 h can be obtained while the NCM523/Li pouch cell demonstrates a high capacity of 760 mAh and 96 % capacity retention after cycling, holding great promises to be utilized for practical solid‐state Li metal batteries.

Facilitating Ion Storage and Transport Pathways by In Situ Constructing 1D Carbon Nanotube Electric Bridges between 2D MXene Interlayers.

Multiple van der Waals (vdW) gaps invoke abundant opportunities for contriving artificial architectures and tailoring desired properties via the intercalation route beyond the reach of conventional concepts. Intriguingly, the electrochemical intercalation strategy can precisely and reversibly tune the intercalation stage of charged functional species. This study presents a valid structural editing protocol facilitated by electrochemical intercalation to engineer MXene interlayers, ultimately incorporating in situ constructed carbon nanotube (CNT) electric bridges for enhanced ion storage and transport pathways. The method allows for the precise modulation of electrochemical forces to tailor materials for specific applications. Deep intercalation and in situ growth processes establish robust anchoring sites and connectivity hubs between MXenes and CNTs, ensuring structural homogeneity and stability in advanced electrode materials. The results demonstrate the effectiveness of electrochemistry-mediated interlayer nanoengineering in MXenes, offering a versatile approach to design vdW heterostructures with tailored functionalities for energy storage and conversion applications. This work highlights the potential of electrochemical modulation in advancing materials engineering strategies for next-generation energy storage technologies.

Facile synthesis of monoclinic (NH4)2V4O9 nanosheets for zinc-ion batteries

Aqueous zinc-ion batteries (ZIBs) are increasingly popular due to their low cost and high safety. However, the quest for cathode materials with robust internal structures and efficient ion transport pathways remains critical. In this study, we introduce a simple hydrothermal method to synthesize monoclinic (NH4)2V4O9 nanosheets, serving as a advanced cathode for ZIBs. This material demonstrates outstanding electrochemical properties, with a high specific capacity of 389 mAh g−1 at 0.1 A g−1, and retains 78.9 % capacity after 3000 cycles at 1 A g−1 and 77.3 % after 15,000 cycles at 5 A g−1. Additionally, it achieves an energy density of 325 Wh kg−1 at 101 W kg−1. In-depth electrochemical analysis reveals the structural stability during reversible Zn2+ ion intercalation/de-intercalation, underscoring the potential of (NH4)2V4O9 as a high-performance material for ZIBs.

Hyperstable low-tortuosity fast ion nanochannels for MXene electrodes

The development of flexible MXene-based electrodes with hyperstable ion nanochannels and low tortuosity, remains daunting challenging for long-term wearable electronic devices. This paper presents a hydrogen-bonding enhanced holey MXene (HC-HMXene) electrode with maximum ion accessibility, optimized ion transport pathways, and hyperstable ion nanochannels. Specifically, three roles of introducing in-plane mesopores, reducing the lateral dimensions, and increasing the interlayer spacing in HMXene film notably enhance the electrolyte permeation efficiency and shorten the ion transport paths of the electrode (resulting in a 78.7-fold decrease in tortuosity). Thus, the constructed HC-HMXene electrode exhibits 41.1 times higher diffusion coefficient and 2.3 times higher specific capacitance than those of closely restacked film electrode with the same mass loading of MXene. Furthermore, the aramid nanofibers introduced among the MXene layers as interlocking agents bond the nanosheets via hydrogen interaction and significantly enhance the stability of the ion channel. Consequently, the HC-HMXene film effectively resists swelling behavior and maintains good structural stability in aqueous media. Moreover, the flexible sensing integrated system, powered by a HC-HMXene-based zinc ion microcapacitor, exhibits promising application prospects in real-time monitoring human physiological characteristics.

Bipolar Membranes Via Divergent Synthesis: On the Interplay between Ion Exchange Capacity and Water Dissociation Catalysis.

Bipolar membranes (BPMs) enable the operation of electrochemical reactors with electrode compartments in different chemical environments or pH. The transport properties at the microscopic scale are dictated by the composition and morphology of the interfacial junctions as well as the specific chemistry of the ion-exchange layers that support the current of protons and hydroxide ions. This work elucidates the relation between water-dissociation efficiency and the physicochemical properties of the individual ion-exchange membrane layers in the poly(styrene-b-poly(ethylene-ran-butylene)-b-polystyrene) (SEBS)-based BPM. The optimal water dissociation performance of three previously reported water-dissociation catalysts in the SEBS-based BPM was examined, with junction thickness of graphene oxide > TiO2 > SnO2, resulting in disparate junction morphologies at the BPM's interface. A hybrid junction system, which included both the effective water dissociation catalyst SnO2 and direct contacting of the ion-exchange membrane layer, exhibited high water dissociation efficiency. This was likely due to the immediate ion transport pathway provided by direct membrane contact around the catalyst, which also improved the interfacial adhesion. A higher ion exchange capacity (IEC) in BPMs substantially enhanced the water dissociation performance in BPMs without water-dissociation catalysts. However, the incorporation of the effective SnO2 catalyst into the BPMs with a lower IEC significantly improved performance, an effect attributed to the hybrid junction system. Additionally, the increase in water uptake and ion conductivity of the cation exchange layer with higher IEC suggested that the cation exchange layer and its interface to the water-dissociation catalyst layer may play a key role in water dissociation. This study identifies the key parameters of individual BPM components and their interactions to water dissociation performance, offering new insights to guide in the construction of future BPMs optimized for enhanced water dissociation efficiency at high current densities.

Indium oxide decorated graphitic carbon nitride/multiwalled carbon nanotubes ternary composite for supercapacitor applications

A hybrid ternary composite In2O3/g-C3N4/MWCNT (GCI) was synthesized by combining three-dimensional In2O3, two-dimensional g-C3N4, and one-dimensional MWCNTs employing a one-pot solvothermal method. The resulting In2O3/g-C3N4/MWCNTs composite leverages the combined benefits of the integration of different dimensionality materials and the synergy between its components. Integrating 1D, 2D, and 3-D materials can create hybrid structures with 3D architectures. It exhibits hierarchical porosity that provides better conductive pathways for ion transport and improves the rate performance. The distinct spatial structure of the composite with short ion diffusion paths maximizes the exposure of the active sites and enhances the conductivity, leading to superior energy storage performance. The electrochemical assessment of the In2O3/g-C3N4/MWCNTs composite exhibited a remarkable specific capacitance of 1081 F g−1 at 1 A g−1 with a commendable capacitance retention of 97.5 % at 3 A g−1 over 5000 cycles. An asymmetric supercapacitor fabricated using In2O3/g-C3N4/MWCNT//AC showcased a notable energy density of 57.5 Wh Kg−1 with an impressive power density of 2760 W Kg−1 at 1 A g−1. The outstanding electrochemical attributes of the fabricated device underscore the potential of the material for future applications in hybrid energy storage systems.

Construction of a Borophene-Based Hybrid Aerogel for Multifunctional Applications.

As a novel approach to pursue high-performance multifunctional materials, the structural design of cutting-edge two-dimensional (2D) materials has ignited substantial interests. Borophene, an emerging member in the realm of 2D materials, exhibits crucial attributes, including high theoretical carrier density, electrical conductivity, magnetism, and high aspect ratio, rendering it highly promising for diverse applications. Yet, the exploration of porous structural configurations of borophene remains untapped. Addressing this gap, our study focuses on the fabrication of a multifunctional borophene hybrid foam (CMB-foam). This hybridization leverages the exceptional multifunctionality of MXene alongside borophene within a three-dimensional porous framework, facilitating reflection and absorption of electromagnetic waves, thereby demonstrating remarkable electromagnetic interference (EMI) shielding capabilities. Moreover, this structural configuration exposes an enlarged surface area, thus shortening the transport pathway for electrolyte ions, leading to an excellent energy storage performance. Additionally, CMB-foam performs well in thermal management and thermal insulation. These findings underscore the potential of borophene-based materials in multifunctional applications and offer valuable insights into further performance explorations in this domain.

Electrospun carbon/iron–vanadium oxide nanofibers for high energy density supercapacitors

Highly flexible and conductive carbon nanofibers (CNFs) embedded with pseudocapacitive iron–vanadium oxide (FVO) nanoparticles were fabricated via electrospinning of a metal salt/polyacrylonitrile solution followed by high-temperature annealing (750 °C). CNFs have a graphitic structure with defects, which could accelerate electron mobility and the access of electrolytic ions to the multivalent FVO nanoparticles, respectively. Poly(methyl methacrylate) (PMMA) was introduced as a sacrificial polymer to alter the internal structure of the nanofibers and thus enhance the electrolytic ion transport pathways. Terephthalic acid was added to provide flexibility by increasing the cross-linking within the electrospun fibers. The flexible FVO/CNFs exhibited excellent electrochemical performance. The optimal sample had a high areal capacitance of 1058 mF·cm−2 at a current density of 2.5 mA·cm−2 and showed 100 % capacitance retention during long-term cycling (10,000 cycles). The capacitance at a high current density of 25 mA·cm−2 was 81.3 % of that at a current density of 2.5 mA·cm−2. Using a wider potential window of 0–1.6 V increased the energy density to 389 μW·h·cm−2. The optimal FVO/CNF sample maintained 90 % of its initial capacitance after 200 bending cycles.

Significantly Enhanced Oxidation Resistance and Electrochemical Performance of Hydrothermal Ti3C2Tx MXene and Tannic Acid Composite for High-Performance Flexible Supercapacitors.

The electrochemical performances of Ti3C2Tx MXene are severely restricted by the easy oxidation and restacking. Herein, tannic acid (TA) is introduced into Ti3C2Tx dispersion, and the mixed dispersion is further subjected to a simple hydrothermal treatment to prepare the hydrothermal Ti3C2Tx and TA composite (h-Ti3C2Tx@h-TA). Due to the decomposition of TA into gallic acid (GA), hydrothermal TA (h-TA) is a mixture of TA and GA. The strong interaction between h-TA and MXene mainly involves chemical interaction between the hydroxyl groups in h-TA and the surface/edge Ti atoms, along with numerous hydrogen bonds. The h-TA intercalation weakens MXene restacking and increases interlayer spacing, thereby improving ion transport pathways and accessibility. The chemical interaction between the hydroxyl groups of GA and the Ti atoms significantly enhances oxidation resistance and pseudocapacitive active sites. Therefore, the h-Ti3C2Tx@h-TA film electrode shows significantly enhanced capacitance (848 F·g-1 at 1 A g-1) and cycling stability (100% retention after 20 000 cycles). Moreover, flexible sandwiched supercapacitors with symmetrical h-Ti3C2Tx@h-TA electrodes exhibit a high energy density of 30.1 Wh kg-1 at a high power density of 300 W kg-1, outperforming those of Ti3C2Tx-based film electrodes and sandwiched supercapacitors reported so far. The extrusion-printed microsupercapacitors with h-Ti3C2Tx@h-TA electrodes demonstrate high areal capacitance (135 mF cm-2 at 5 mV s-1) along with energy storage performance (6.74 μWh cm-2 at 506 μW cm-2) and cycling stability (98.8% retention after 41 460 cycles), all while maintaining excellent flexibility. These impressive results indicate the great application potential of the hydrothermal Ti3C2Tx MXene and tannic acid composite in flexible energy storage devices.

Highly Anion-Conductive Viologen-Based Two-Dimensional Polymer Membranes as Nanopower Generators.

Two-dimensional polymers (2DPs) and their layer-stacked 2D covalent organic frameworks (2D COFs) membranes hold great potential for harvesting sustainable osmotic energy. The nascent research has yet to simultaneously achieve high ionic flux and selectivity, primarily due to inefficient ion transport dynamics. This is directly related to ultrasmall pore size (<3 nm), much smaller than the duple Debye length in the diluted electrolyte (6-20 nm), as well as low charge density (<4.5 mC m-2). Here, we introduce a π-conjugated viologen-based 2DP (V2DP) membrane possessing a large pore size of 4.5 nm, strategically enhancing the overlapping of the electric double layer, coupled with an exceptional positive surface charge density (~6 mC m-2). These characteristics enable the membrane to facilitate high anion flux while maintaining ideal selectivity. Notably, V2DP membranes realize an impressive current density of 5.5×103 A m-2, surpassing benchmarks set by previously reported nanofluidic membranes. In the practical application scenario involving the mixing of artificial seawater and river water, the V2DP membranes exhibit a considerable ion transference number of 0.70 towards Cl-, contributing to an outstanding power density of ~55 W m-2. Theoretical calculations reveal the important role of the large quantity of anion transport sites, which act as binding sites evenly located in the positively charged N-containing pyridine rings. These binding sites enable kinematic coupling and decoupling between anions and the V2DP skeleton, establishing a continuous Cl- ion transport pathway. This work demonstrates the great promise of large-area ultrathin 2DP membranes featuring highly organized charged ion transport networks when applied for osmotic energy conversion.

MOF-on-MOF Derived Co2P/Ni2P Heterostructures for High-Performance Supercapacitors.

Metal-organic frameworks (MOFs) have been widely used as versatile precursors to fabricate functional nanomaterials with well-defined structures for various applications. Herein, the presynthesized Ni-MOF nanosheets were grown on a Ni foam (NF) substrate, which then guided the nucleation and further growth of Prussian blue analogues (PBA) nanocubes to form MOF-on-MOF of the PBA/Ni-MOF film. This film was subsequently converted into a Co2P/Ni2P heterostructure. The NF-supported Co2P/Ni2P composites exhibited excellent supercapacitor performance, delivering a high specific capacity of 5124.2 mF cm-2 at 1 mA cm-2 and a remarkable capacity retention of 80.69% after 3000 cycles at 10 mA cm-2. An asymmetric supercapacitor assembled using Co2P/Ni2P/NF as the cathode and activated carbon as the anode yielded a maximum energy density of 0.34 mWh cm-2 at a power density of 1.50 mW cm-2. The enhanced supercapacitor performance is attributed to the synergistic effects of the Ni2P and Co2P components with multiple valence states as well as the unique hierarchical structure, which provides efficient pathways for electron and ion transport while mitigating volume expansion during energy storage. This synthetic strategy demonstrates an effective approach to fabricate phosphide-based hybrid materials for high-performance supercapacitor applications.

Preparation and Conductivity Analysis of LLTO Nanofiber‐Incorporated PEO‐PVDF‐HFP‐LiClO4 Solid Polymer Electrolytes for High‐Voltage Lithium Metal Batteries

ABSTRACTThis work focuses on the development of a composite polymer electrolyte (CPE) for all‐solid‐state lithium metal batteries (ASSLMBs), integrating LLTO nanofibers into a PEO (polyethylene oxide)‐PVDF‐HFP (poly(vinylidene fluoride‐cohexafluoropropylene)) matrix with LiClO4 as the lithium salt. The PEO has high ionic conductivity and flexibility, and the PVDF‐HFP has high mechanical strength and electrochemical stability. Therefore, the resulting composite has improved electrochemical performance and mechanical properties. Incorporating LLTO nanofibers enhances ionic conductivity due to the one‐dimensional ion transport pathways provided by the nanofibers while maintaining mechanical integrity and air stability, overcoming the challenges associated with conventional fillers. The prepared CPE demonstrates exceptional electrochemical stability up to 5.1 V versus Li/Li+, making it suitable for high‐voltage applications over traditional polymer electrolytes. The optimized CPE with 15 wt% LLTO provides the ionic conductivity of 1.1 × 10−5 S cm−1 at room temperature and reaches 1.46 × 10−4 S cm−1 at 80°C. The assembled LiNi1/3Mn1/3Co1/3PO4||PEO‐PVDF‐HFP‐LiClO₄‐LLTO||Li based 2032 coin cell worked in between 3 and 4.8 V versus Li/Li+ potential window without any electrolyte decomposition from 0.5 to 5 mV/s scan rates. Similarly, the fabricated LiFePO₄||PEO‐PVDF‐HFP (1:2)‐LiClO4‐LLTO (15 wt%)||Li cell provides an initial capacity of 149 mAh g−1 at 0.1 C and 85 mAh g−1 at 0.5 C, exploring its potential for lithium metal batteries. Overall, this work offers a promising pathway for developing advanced solid polymer electrolytes for next‐generation lithium metal batteries, which combine high ionic conductivity, excellent electrochemical performances, and robust mechanical properties.

Nanofibers endow NASICON-type Na3.3La0.3Zr1.7Si2PO12 electrolyte/Na4MnCr(PO4)3 cathode excellent electrochemical properties

All-solid-state sodium-ion batteries (ASSSIBs) using composite polymer electrolytes (CPEs) are promising candidates for addressing the high cost, safety issues, and limited energy density of traditional lithium-ion batteries. The microstructure and morphology of active ceramic filler and cathode seriously affect the construction of ion/electron transport channels and electrochemical performance, while the contact tightness at the electrode/CPE interface determines the release of energy storage performance in ASSSIBs. Here, NASICON-type Na3.3La0.3Zr1.7Si2PO12 (NLZSP) ceramic nanofibers (NFs) and Na4MnCr(PO4)3@C (NMCP@C) NFs are prepared via electrospinning. NLZSP long NFs (L-NFs) can be uniformly dispersed in PVDF-HFP using ultrasonic treatment to create rapid ion transport pathways within the ceramic and polymer/ceramic interphases, enabling the CPE to achieve high ionic conductivity of 3.36 × 10−4 S·cm−1, wide electrochemical stability window (ESW) exceeding 5 V, low activation energy (Ea) of 0.28 eV and sodium-ion transference number (TNa+) of 0.65 at room temperature. Meanwhile, NMCP@C NFs can enhance electron conductivity and reduce the sodium ion migration path, and finally achieve a superhigh specific capacity (161 mAh·g−1) and energy density (534 Wh·kg−1) at 0.1C. Additionally, the integrated NMCP@C/CPE structure is incorporated into NMCP@C/CPE//Na solid state sodium metal batteries (SMBs), which exhibits excellent rate performance and high capacity retention of 78.8 % at 1C (1.4–4.3 V) and 70.5 % at 0.5C (1.4–4.6 V) after 200 cycles. This study offers valuable insights into constructing high-performance ASSSIBs.

Edge‐Enriched MoS2 as a High‐Performance Cathode for Aqueous Zn‐Ion Batteries

AbstractRechargeable aqueous zinc ion batteries (AZIBs) with the advantages in low cost, high safety, and environmental friendliness have broad application prospects in the field of energy storage. However, the slow diffusion kinetics of multivalent Zn2+ in materials make it hard to find a suitable cathode. Herein, HNO3 etched MoS2 with edge‐enriched feature is proved to be a promising cathode for high‐performance AZIBs. The highly exposed edges with superior electrochemical activity can not only offer more reactive sites for zinc storage but also facilitate electrolyte accessibility and shortens the ion transport pathway, thus accelerating reaction kinetics. As a result, the edge‐enriched MoS2 cathode exhibited higher specific capacity of 187 mAh g−1 at 0.1 A g−1 and outstanding cycling performance (89 % capacity retention after 700 cycles at 1 A g−1).

Two-dimensional heterostructure of MXene-derived V2O5·H2O and graphene with enhanced Zn-ion storage capability

Aqueous rechargeable zinc-ion batteries (ZIBs) are promising candidates for gird-scale energy storage with economic and environmental advantages. Layered hydrated vanadium oxides with multivalent and “lubricating” effect receive much attention in ZIBs. However, the application of them is suffering from the poor intrinsic conductivity and the unstable structure. Herein, a unique 2D/2D heterostructure of δ-V2O5·H2O nanobelts (VO) and reduced graphene oxide (rGO) is designed as cathode for ZIBs (denoted as VOG). The stronger interface coupling and the shorter ion transport pathways impart the VOG electrode impressive stability and fast ions diffusion kinetics. Specifically, the VOG cathode delivers a superior capacity of 342 mAh g−1 at 1 A g−1 and a remarkable rate capability of 280 mAh g−1 at a quite high rate of 10 A g−1. The energy storage mechanism involved is investigated by systematical characterizations. The exploration of such 2D/2D heterostructure materials with strong synergy sheds light on the rational design of high performanced AZIBs.