Cathode For Zinc-ion Batteries Research Articles

Facile synthesis of V2O3@C nanoribbons by rapid cooling method for high-capacity zinc-ion batteries cathode

Aqueous zinc-ion batteries (ZIBs) have recently gained considerable attention due to their low price and great safety properties. However, the challenge of preparing high-performance cathode materials and developing low-cost, efficient preparation methods still demands urgent solutions. Herein, this paper proposes the use of a rapid cooling method to prepare V2O3@C cathode materials with excellent overall electrochemical performance for ZIBs. Utilizing low-cost ammonium metavanadate as the raw material and melamine as a binding agent, dispersed molecules facilitate the rapid creation of V-based nanoribbon precursors within just 1 h at a low temperature. After the annealing process, the obtained V2O3@C nanoribbons exhibit a unique structural architecture with a V2O3 covered by carbon, providing enhanced structural stability and electric conductivity. In contrast to the commercial V2O3 cathode, the V2O3@C cathode exhibits remarkably improved electrochemical characteristics, including enhanced specific capacity (41 % increase), extended cycle stability (capacity retention of 63 % after 15,000 cycles), and improved rate capability (53 % capacity retention at 10 A g−1). Additionally, the zinc storage mechanism of the V2O3@C cathode was systematically investigated. This facile synthesis method, coupled with the outstanding electrochemical performance, highlights the potential of V2O3@C cathode as a promising candidate for high-capacity cathodes in next-generation ZIBs.

A Cu/MnOx Composite with Copper-Doping-Induced Oxygen Vacancies as a Cathode for Aqueous Zinc-Ion Batteries.

Aqueous zinc-ion batteries are anticipated to be the next generation of important energy storage devices to replace lithium-ion batteries due to the ongoing use of lithium resources and the safety hazards associated with organic electrolytes in lithium-ion batteries. Manganese-based compounds, including MnOx materials, have prominent places among the many zinc-ion battery cathode materials. Additionally, Cu doping can cause the creation of an oxygen vacancy, which increases the material's internal electric field and enhances cycle stability. MnOx also has great cyclic stability and promotes ion transport. At a current density of 0.2 A g-1, the Cu/MnOx nanocomposite obtained a high specific capacitance of 304.4 mAh g-1. In addition, Cu/MnOx nanocomposites showed A high specific capacity of 198.9 mAh g-1 after 1000 cycles at a current density of 0.5 A g-1. Therefore, Cu/MnOx nanocomposites are expected to be a strong contender for the next generation of zinc-ion battery cathode materials in high energy density storage systems.

Tailored thickness engineering of Bi2Se3 nanosheets for superior cathodic performance in aqueous zinc-ion batteries

Bi2Se3 is considered a suitable cathode material for zinc-ion batteries (ZIBs) because of its high conductivity and large layer spacing. Herein, Bi2Se3 nanosheets with varying thicknesses are successfully synthesized using a one-step solvothermal process with adding different amounts of ethylenediamine. The introduction of ethylenediamine reduces the thickness of Bi2Se3 from 250 nm to 22.7 nm. The thin structure exposes more active sites and shortens ion transport paths. Therefore, the optimized Bi2Se3 nanosheet exhibits outstanding specific capacity (410 mA h g−1 at 0.2 A/g), high-rate performance (230 mA h g−1 at 5 A/g), and remarkable cycling stability (82.3 % capacity retention after 1200 cycles at 5 A/g). Furthermore, an in-depth exploration of cathodes during cycling is conducted to investigate the charge/discharge mechanism. A dynamic phase transition from Bi2Se3 to BiSe, accompanied by nanosheet exfoliation, is observed during the initial few cycles, designating BiSe as the primary active material. Moreover, an additional redox reaction involving multiple electrons has been proposed. This study offers a valuable guidance for utilizing Bi2Se3 as a cathode in ZIBs.

Synergy of structural engineering and VO2 self-transformation enables ultra-high areal capacity cathodes for zinc-ion batteries

The development of cathodes with high areal capacities is a prerequisite for realizing the practical application of zinc-ion batteries (ZIBs). However, the slow ion (de)intercalation kinetics and the highly tortuous ion transport channels in the traditionally blade-coated electrodes limit the practical areal capacities of the ZIB cathodes below 3 mAh cm−2. In this work, multi-stage pore structures, including through-holes perpendicular to the electrode and submicron-scale channels along the radial direction of the printed filaments, are obtained through polyvinylidene difluoride (PVDF) phase separation assisted 3D printing procedure. In this novel electrode material, the porous network enables fast electron/ion transport and improves the accessibility of active materials for thick electrodes with high active material loadings. More importantly, a phase self-transformation of VO2 to a high oxidation state of V5O12∙6H2O is achieved by regulating the charging voltage, which significantly enhances the zinc storage capacity and provides smoother channels for fast ion (de)intercalation. With these unique features, the 3D printed VO2 cathode with a mass loading of 8.9 mg cm−2 demonstrates a high specific capacity of 478.1 mAh g−1 at 1 A g−1 and a stable life cycle for 1000 cycles at 4 A g−1. When the mass loading is increased to 29.6 mg cm−2, the electrode is still able to deliver an ultra-high areal capacity of 16.8 mAh cm−2. The strategies adopted in this work greatly boost up the performance of VO2 cathodes, especially the high areal capacity, by combining structural engineering and material activity regulation.

Co-insertion of K+ and Ca2+ in vanadium oxide as high-performance aqueous zinc-ion battery cathode material

Inserting metal ions into vanadium oxides can effectively improve their electrochemical properties, and the insertion of different single metal ions into vanadium-based compounds can enhance their electrochemical performance in different ways. Moreover, the insertion of multiple metal ions into vanadium-based compounds may provide a synergistic effect. Therefore, in this work a K0.02Ca0.18V2O5·0.7H2O (KCaVOH) cathode material was obtained by co-inserting the monovalent metal ion K+ and the divalent metal ion Ca2+ into vanadium oxide through a one-step hydrothermal method. The insertion of K+ enhances the structural stability of the cathode material, while the insertion of Ca2+ increases the layer spacing between the V-O layers and improves the specific capacity of the cathode material. The co-insertion of K+ and Ca2+ effectively enhances the electrochemical performance of V2O5·1.6H2O, and the KCaVOH cathode provides a high specific capacity of 410 mAh·g−1 at 0.3 A·g−1. Moreover, the capacity still reaches 265 mAh·g−1 after 1800 cycles at 5 A·g−1. This method provides a strategy for significantly enhancing the electrochemical performance of vanadium-based cathode materials.

Enhancing the electrochemical activation kinetics of V2O3 for high-performance aqueous zinc-ion battery cathode materials

The discharge capacity and lifespan of zinc ion batteries currently remain impractical due to limitations in the cathode. Low-valence vanadium oxides are promising cathode material precursors that can be electrochemically converted into highly active hydrated amorphous oxides. However, the activation process itself suffers from structural instability or high local strain, due to the low electronic conductivity and the limited ion diffusion kinetics. To tackle this issue, herein, we synthesize porous carbon-coated nitrogen-doped V2O3 (p-NVO@C) microparticles utilizing a nitrogen-containing vanadium-based metal–organic framework (MOF) as the precursor. The uniform N doping and carbon coating improve the electronic conductivity of the active material particles. The carbon coating also traps the active material to reduce its dissolution loss; the high porosity of the p-NVO@C alleviates the stress from Zn2+-intercalation-induced expansion and shortens the ion transport paths. Moreover, first-principles calculations indicate that the doped N atoms in vanadium oxides generate a locally enhanced electric field, which accelerates the diffusion of Zn2+. Given the above advantages, the p-NVO@C particles demonstrate an outstanding specific capacity of 501 mAh/g at a current density of 0.2 A/g and a remarkable rate performance after the initial activation. The capacity retention rate remains as high as 95.7 % after 2000 cycles at a current density of 10 A/g. Ex-situ characterizations confirm the robust structural stability during phase transition cycles. This work provides an excellent solution to developing cathode materials for high-performance aqueous zinc ion batteries.

The effect of copper doping in α-MnO2 as cathode material for aqueous Zinc-ion batteries

Copper-doped Manganese Dioxide has been synthesised through a simple hydrothermal method at different doping levels. The synthesised materials have been characterized by X-ray diffraction (XRD), and scanning electron microscopy (SEM) to determine the composition, structure, and morphology. All the Cu doped MnO2 are found to be single phased. Their electrochemical properties as cathode for Zinc-ion batteries are studied by cyclic voltammetry (CV), galvano-static charge / discharge (GCD) and electrochemical impedance spectroscopy (EIS), using 3 M ZnSO4 + 0.3 MnSO4 solution as the electrolyte. 3.8% Cu doped MnO2 has shown the highest initial capacity of 379.5 mAh g−1 at 0.02 A·g−1, and 304.4 mA h g−1 at 0.5 A g−1, but experienced fast fading with a poor capacity retention of 56.8% after 100 cycles. 7.4% Cu doping gives lower capacity, while 5.9% doping shows a higher discharging capacity (320.0 mAh·g−1 at 0.02 A·g−1 and 269.3 mAh·g−1 at 0.5 A·g−1) and improved stability (85.8% capacity retention after 100 cycles), better than non-doped MnO2 electrode (284.4 mAh g−1 at 0.02 A g−1 and 252.1 mAh·g−1 at 0.5 A g−1, capacity retention 76.7%). The samples show satisfactory capacity and rate capability while the cycling stability is not ideal, which may relate to the needle like morphology and nanoscale particle size. CV tests revealed that the electrochemical process is mainly diffusion controlled. The zinc ion diffusion coefficient is tested to be in the range of 10−12 cm2·s−1 from both CV and EIS tests and showed the same trend in their electrochemical capacity. Doping of Copper in MnO2 reduced the polarization on electrode, improved the electrochemical reversibility, as evidenced by the reduction of the redox peak potential difference from 0.31 to 0.24 V at 1.1 mV·s−1, and from 0.45 V to 0.31 V at 5 mV·s−1. Whilst the cell resistance of non-doped MnO2 increased from 1.78 Ω to 7.39 Ω after cycling, the cell resistances of all Cu-doped cathodes reduced, indicating improved electronic conductivities after cycling. These results indicate that Cu-doping is effective to increase the conductivity of the materials, reduce the polarization during charge and discharge, and improve the cycling stability of MnO2 cathode.

Recent development in addressing challenges and implementing strategies for manganese dioxide cathodes in aqueous zinc ion batteries

Recent development in addressing challenges and implementing strategies for manganese dioxide cathodes in aqueous zinc ion batteries

Bimetallic Intercalated Vanadium Oxide As a High-Performance Cathode for Aqueous Zinc Ion Batteries.

In this paper, a bimetallic Na0.13Mg0.02V2O5·0.98H2O (NMVO) material with an interlayer spacing of 11.67 Å was synthesized by a simple preintercalation method as a cathode for zinc ionic batteries (ZIBs). The large layer spacing provides a wide channel for the embedding of Zn2+, resulting in high reversible capacity and ion diffusion kinetics. In addition, by virtue of the high electronic conductivity of metal ions, NMVO exhibits excellent electronic conductivity under the combined action of Na+ and Mg2+ bimetallic intercalation. At the same time, preintercalation ions and structural water act as interlayer pillars to stabilize the layer structure of NMVO during the cycling process. The above reasonable structural design endows the NMVO with excellent electrochemical performance. The battery with NMVO cathode delivers a high initial capacity of 126 mAh g-1 at 10 A g-1, and still remains at 76% after 5000 cycles, providing 100 Wh kg-1 energy density and 9.5 kW kg-1 power density (based on the mass of cathode). This bimetallic intercalation structure provides a general feasible scheme for the design of vanadium-based electrode materials.

High conductive poly(1,8-diaminonaphthalene)/graphene nanocomposite as a cathode for zinc ion batteries

Recently, aqueous zinc ion batteries (AZIBs) are experiencing rapid development benefiting to their high safety and increasing electrochemical performance. Among all kinds of AZIB electrode materials, organic materials have attracted attentions due to their unique advantages such as structural flexibility, small volume expansion, abundant Zn2+ storage sites and environmental friendliness. However, issues involving electrode dissolution, sluggish electrochemical kinetics etc. still hampered the prior choice of organic electrodes. Herein, we designed a poly(1,8-diamino-naphthalene)/ graphene composite aiming to improve the availability of organic electrodes in AZIBs. By means of constructing high conducting graphene network and the synergetic effect between the two components, the electronic transfer kinetics and overall electrochemical performance of PDAN organic electrode have been fully improved. The organic-inorganic composite exhibited an initial specific capacity of 240 mA·h·g−1 and stable galvanostatic cycling after 1000 cycles, exceeding the original polymer.

One-Stone-for-Two-Birds Strategy for VSe2 to Enable High Capacity and Long-Life Zinc Storage.

Based on a specific zinc storage mechanism and excellent electronic conductivity, transition metal dichalcogenides, represented by vanadium diselenide, are widely used in aqueous zinc-ion battery (AZIB) energy storage systems. However, most vanadium diselenide cathode materials are presently limited by low specific capacity and poor cycling life. Herein, a simple hydrothermal process has been proposed for obtaining a vanadium diselenide cathode for an AZIB. The interaction of defects and crystal planes enhances zinc storage capacity and reduces the migration energy barrier. Moreover, abundant lamellar structure greatly increases reaction sites and alleviates volume expansion during the electrochemical process. Thus, the as-obtained vanadium diselenide AZIB exhibits an excellent reversible specific capacity of 377 mAh g-1 at 1 A g-1, and ultralong cycle stability of 291 mAh g-1 after 3200 cycles, with a nearly negligible capacity loss. This one-stone-for-two-birds strategy would be expected to be applied to large-scale synthesis of a high-performance zinc-ion battery cathode in the future.

Metal ions and organic molecule co-intercalated vanadium oxide cathode for high-performance zinc-ion batteries

Vanadium oxide is a highly promising cathode material for zinc-ion batteries due to its unique layered structure and high theoretical capacity. However, the material dissolution and structural collapse severely limit the development of zinc-ion batteries. Herein, inorganic metal ions (Mg2+) and organic polymer molecules (PANI) were introduced into the hydrated vanadium oxide interlayer in this paper. Mg2+ ions enhance the conductivity of the cathode and widen the interlayer spacing. Meanwhile, PANI serves to cushion the structural expansion resulting from ion embedding and stabilize the layered structure. Additionally, PANI actively participates in the charging and discharging process, thereby enhancing the diffusion rate of Zn2+. Thanks to the synergistic effect of Mg2+ and PANI, the MgVOH/PANI cathode exhibits a discharge capacity of 412 mAh·g−1 at 0.1 A g−1 and retains 93% of its capacity after 1000 cycles at a current density of 2A·g−1. This synergistic strategy of combining organic molecules and inorganic ions can provide a reference for improving the kinetic and structural stability of other aqueous battery cathodes.

Enhanced electrochemical energy storage devices utilizing a one-dimensional (1D) α-MnO2 nanocomposite encased in onion-like carbon

AbstractThis work describes the fabrication of a novel one-dimensional (1D) α-MnO2 nanorods encased in onion-like carbon (or) carbon nano-onions (OLC) via microwave irradiation techniques employing electrolytic manganese dioxide (EMD), which is especially beneficial for rapid ion and electron transfer, and great structural stability. The composite of α-MnO2 and OLC demonstrates exceptional performance as an electrode across various electrochemical energy storage systems, including zinc-ion batteries (ZIB), sodium-ion batteries (SIB), and supercapacitors (SC) than the pristine α-MnO2. In SIB systems, the composite exhibits a specific capacity of 266 mAh g−1 at initial cycle with 50% capacity retention over 500 cycles, whereas the pristine electrode delivers only 39% capacity retention. The rapid yet controlled charge transfer kinetics facilitated by OLC addition in the α-MnO2 matrix outperforms as the ZIB cathode with an excellent specific capacity of 476 mAh g−1 with 100% capacity retention, while the pristine sample exhibits 77.5% capacity retention. As a SC electrode, the α-MnO2/OLC composite exhibits better electrochemical properties such as rectangular behavior, increased specific capacitance (792 F g−1), excellent capacity retention at high current densities, and others. The higher surface area that could be offered by the OLC to the α-MnO2 matrix facilitates the improved electrochemistry in the pristine sample and this kind of modification can be a viable solution to overcome the limitations of α-MnO2 for electrochemical energy storage applications. It is important to note that the performance outputs of α-MnO2/OLC composite are far better than the regular carbon (graphite, graphene) in α-MnO2 electrodes. Further, OLC provided with high surface area and ordered morphology can play the role of conductivity booster, structural stabilizer, and electrochemical active material in all the energy storage applications which may give a significant research attention in near future.

Tunnel-Oriented VO2 (B) Cathode for High-Rate Aqueous Zinc-Ion Batteries.

Tunnel-type vanadium oxides are promising cathodes for aqueous zinc ion batteries. However, unlike layer-type cathodes with adjustable layer distances, enhancing ion-transport kinetics in tunnels characterized by fixed sizes poses a considerable challenge. This study highlights that the macroscopic arrangement of the electrode crucially determines tunnel orientation, thereby influencing ion transport. By changing the material morphology, the tunnel orientation can be optimized to facilitate rapid ion diffusion. In a proof-of-concept demonstration, it is revealed that (00l) facets-dominated VO2 (B) nanobelts with dispersive morphology (VO2-D) tend to adopt a stacking pattern with directional ion transport along the c-axis on the electrode and guarantee fast ion diffusion. Compared with the aggregated sample (VO2-A) that tends to random arrangement on the electrode with isotropic and slow ion transfer behavior, the electrode featuring dispersive (00l) facets-dominated VO2 (B) nanobelts displays directional and fast ion diffusion behavior, thus exhibits an ultrahigh-rate performance (420.8 and 344.8 mAh g-1 at 0.1 and 10 A g-1, respectively) and long cycling stability (84.3% capacity retention under 5000 cycles at 10 A g-1). The results suggest that simultaneous manipulation of exposed crystal facet and morphology-related electrode arrangement should be promising for boosting the ion-transport kinetics in tunnel-type vanadium oxide cathodes.

Heat activated VO2 (R) cathodes for high-performance aqueous zinc ion batteries

We introduce a novel approach for design and production of vanadium dioxide (VO2) cathodes activated by heat, specifically tailored for use in aqueous zinc-ion batteries (ZIBs). Our cathodes exhibit distinctive metal-insulator transition (MIT) characterized by the shift between monoclinic (M) and tetragonal rutile (R) phases. The employment of an aqueous electrolyte in ZIBs enables successful operation of VO2 cathodes, showcasing phase transition and enhanced electrochemical performance above a readily attainable temperature of approximately 68 °C. The MIT feature enhances the charge transfer properties at electrode-electrolyte interfaces, resulting in notable improvements in specific capacity and energy densities. Fabricated VO2(M) cathodes underwent heat-triggered transformation to VO2(R), resulting in a remarkable increase (400 %) in capacity. At 0.1 A g−1, VO2(R) cathodes show specific capacity of 354.6 mAh g−1, yielding an impressive energy density of 461.0 Wh kg−1 for aqueous ZIBs. This exceptional performance can be attributed to abrupt change in electrical conductivity upon thermal activation of MIT. This work underscores pivotal role of thermally activated MIT in finely tuning electrochemical performance of energy storage systems, prospecting a promising avenue for further advancements.

2D Conductive Metal-Organic Frameworks Based on Tetraoxa[8]circulenes as Promising Cathode for Aqueous Zinc Ion Batteries.

Aqueous zinc-ion batteries (ZIBs) are the new generation electrochemical energy storage systems. Recently, two-dimensional conductive metal-organic frameworks (2D c-MOFs) are attractive to serve as cathode materials of ZIBs due to their compositional diversity, abundant active sites, and excellent conductivity. Despite the growing interest in 2D c-MOFs, their application prospects are still to be explored. Herein, a tetraoxa[8]circulene (TOC) derivative with unique electronic structure and interesting redox-active property are synthesized to construct c-MOFs. A series of novel 2D c-MOFs (Cu-TOC, Zn-TOC and Mn-TOC) with different conductivities and packing modes are obtained by combining the linker tetraoxa[8]circulenes-2,3,5,6,8,9,11,12-octaol (8OH-TOC) and corresponding metal ions. Three c-MOFs all exhibit typical semiconducting properties, and Cu-TOC exhibits the highest electrical conductivity of 0.2 S cm-1 among them. Furthermore, their electrochemical performance as cathode materials for ZIBs have been investigated. They all performed high reversible capacity, decent cycle stability and excellent rate capability. This work reveals the key insights into the electrochemical application potential of 2D c-MOFs and advances their development as cathode materials in ZIBs.

One-Step Hydrothermal Synthesis of NVO Cathodes with Varied Lattice NH4 + Content: Effect on Structural Evolution and Electrochemical Performance.

Aqueous zinc ion batteries have been extensively researched due to their distinctive advantages such as low cost and high safety. Vanadium oxides are important cathode materials, however, poor cycle life caused by vanadium dissolution limits their application. Recent studies show that the lattice NH4 + in vanadium oxides can act as a pillar to enhance structural stability and play a crucial role in improving its cycling stability. Nevertheless, there is still a lack of research on the effect of the lattice NH4 + content on structural evolution and electrochemical performance. Herein, we synthesize vanadium oxides with different contents of lattice NH4 + by a one-step hydrothermal reaction. The vanadium oxides with lattice NH4 + exhibit high initial capacity, as well as good cycling stability and rate performance compared to bare vanadium oxide. Combined with electrochemical analyses, ex-situ structural characterizations, and in-situ X-ray diffraction tests, we reveal that the lattice NH4 + content plays a positive role in vanadium oxides' structural stability and cation diffusion kinetics. This work presents a direction for designing high-performance vanadium cathodes for aqueous zinc ion batteries.

Optimizing Mn in Prussian blue analogs with double redox active sites to induce boosted Zn2+ storage

Prussian Blue analogs (PBAs) are a suitable aqueous zinc-ion batteries (AZIBs) cathode material, but they face issues related to low specific capacity and cycling lifespan due to insufficient active sites and poor ion de-intercalation structural stability. In this study, Mn-Prussian Blue Analog (Mn-PBA) is fabricated using a simple co-precipitation method and the morphology of Mn-PBA is further optimized through artificially manipulating concentration gradients strategy, effectively enhancing the structural stability of Zn2+ de-intercalation. Furthermore, the introduction of Mn established dual Zn2+ active centers in Mn-PBA (Mn-O and Fe(CN)6]4−/[Fe(CN)6]3−), leading to an increased specific capacity. As a proof of concept for AZIBs, the optimized Mn-PBA-3 cathode exhibits a high reversible specific capacity of 143.5 mAh/g and maintains a capacity retention of 88.5 % after 250 cycles at 1 A/g, surpassing commercial MnO2 (30.5 mAh/g after 100 cycles). Mn-PBA-3 also delivers a high capacity of 79.0 mA h g−1 after 2000 cycles of 10 A/g. The mechanism of the Zn2+ double redox reaction of Mn-PBA-3 has been revealed in detail by in situ Raman and a series of ex situ techniques. Under a high operating voltage window of 0–1.9 V, Zn//Mn-PBA-3 demonstrates a capacity of 99.3 mAh/g after 800 cycles (5 A/g) by assembling zinc ion button battery. This work has reference significance for structurally modulated PBAs used in high performance AZIBs.

Highly Electrically Conductive Polyiodide Ionic Liquid Cathode for High-Capacity Dual-Plating Zinc-Iodine Batteries.

Zinc-iodine batteries are one of the most intriguing types of batteries that offer high energy density and low toxicity. However, the low intrinsic conductivity of iodine, together with high polyiodide solubility in aqueous electrolytes limits the development of high-areal-capacity zinc-iodine batteries with high stability, especially at low current densities. Herein, we proposed a hydrophobic polyiodide ionic liquid as a zinc-ion battery cathode, which successfully activates the iodine redox process by offering 4 orders of magnitude higher intrinsic electrical conductivity and remarkably lower solubility that suppressed the polyiodide shuttle in a dual-plating zinc-iodine cell. By the molecular engineering of the chemical structure of the polyiodide ionic liquid, the electronic conductivity can reach 3.4 × 10-3 S cm-1 with a high Coulombic efficiency of 98.2%. The areal capacity of the zinc-iodine battery can achieve 5.04 mAh cm-2 and stably operate at 3.12 mAh cm-2 for over 990 h. Besides, a laser-scribing designed flexible dual-plating-type microbattery based on a polyiodide ionic liquid cathode also exhibits stable cycling in both a single cell and 4 × 4 integrated cell, which can operate with the polarity-switching model with high stability.

Molecular Connectors Boosting the Performance of MoS2 Cathodes in Zinc-Ion Batteries.

Zinc-ion batteries (ZIBs) are promising energy storage systems due to high energy density, low-cost, and abundant availability of zinc as a raw material. However, the greatest challenge in ZIBs research is lack of suitable cathode materials that can reversibly intercalate Zn2+ ions. 2D layered materials, especially MoS2 -based, attract tremendous interest due to large surface area and ability to intercalate/deintercalate ions. Unfortunately, pristine MoS2 obtained by traditional protocols such as chemical exfoliation or hydrothermal/solvothermal methods exhibits limited electronic conductivity and poor chemical stability upon charge/discharge cycling. Here, a novel molecular strategy to boost the electrochemical performance of MoS2 cathode materials for aqueous ZIBs is reported. The use of dithiolated conjugated molecular pillars, that is, 4,4'-biphenyldithiols, enables to heal defects and crosslink the MoS2 nanosheets, yielding covalently bridged networks (MoS2 -SH2) with improved ionic and electronic conductivity and electrochemical performance. In particular, MoS2 -SH2 electrodes display high specific capacity of 271.3 mAh g-1 at 0.1 A g-1 , high energy density of 279Whkg-1 , and high power density of 12.3 kW kg-1 . With its outstanding rate capability (capacity of 148.1 mAh g-1 at 10 A g-1 ) and stability (capacity of 179 mAh g-1 after 1000 cycles), MoS2 -SH2 electrodes outperform other MoS2 -based electrodes in ZIBs.