Excellent Electrochemical Performance Research Articles

A Universal Interfacial Reconstruction Strategy Based on Converting Residual Alkali for Sodium Layered Oxide Cathodes: Marvelous Air Stability, Reversible Anion Redox, and Practical Full Cell.

Mn-based layered oxide cathodes have attracted widespread attention due to high capacity and low cost, however, poor air stability, irreversible phase transitions, and slow kinetics inhibit their practical application. Here, we propose a universal interfacial reconstruction strategy based on converting residual alkali to tunnel phase Na0.44MnO2 for addressing the above mentioned issue simultaneously, using O3 NaNi0.4Fe0.2Mn0.4O2@2 mol % Na0.44MnO2 (NaNFM@NMO) as the prototype material. The optimized material exhibits an initial capacity and energy density comparable with lithium-ion batteries. The reversible anionic redox behavior and charge compensation mechanism of NaNFM@NMO were analyzed and verified by soft X-ray absorption spectrum and in situ X-ray absorption spectrum. Due to the intrinsic stability of the tunnel structure, excellent air stability and highly reversible structure evolution of the NaNFM@NMO cathode material are achieved, which are confirmed by contact angle test, rigorous aging test, and in situ X-ray diffraction. More importantly, the NaNFM@NMO cathode demonstrates a great match with the nonpresodiated hard carbon anode and shows excellent electrochemical performance of the full cell. Additionally, such a strategy could be also applied to modify P2-type cathodes, showing superior universality and good prospects in industrialized production. Overall, the proposed strategy could improve air stability while remaining interfacial and bulk stable simultaneously and will open up a whole new field for the optimization of other electrode materials.

Regulating Li2S Deposition and Accelerating Conversion Kinetics through Intracavity ZnS toward Low-Temperature Lithium-Sulfur Batteries.

The uncontrolled deposition behavior and sluggish conversion kinetics of the discharging product (solid Li2S) severely deteriorate the electrochemical performance of lithium-sulfur (Li-S) batteries, especially under high S loading and low-temperature conditions. Herein, a multifunctional S cathode host consisting of ZnS nanoparticles (NPs) confined in hollow porous carbon spheres (ZnS@HPCS) is synthesized via a unique capillary force-driven melting-diffusion strategy. The porous carbon shell of ZnS@HPCS provides a space-confined reservoir for soluble polysulfides and solid Li2S, while the intracavity ZnS NPs trap polysulfides, induce Li2S inside deposition, and accelerate conversion kinetics. Thus, Li-S batteries with ZnS@HPCS-S cathodes exhibit excellent electrochemical performance at both room and low temperatures (-40 °C) and high reversible capacities under high S loading (5.2 mg cm-2). Furthermore, Li2S nucleation/deposition, in situ Raman, and theoretical analyses reveal the underlying mechanism. This work offers fundamental insights into regulating Li2S deposition and designing S hosts for high-performance Li-S batteries.

Innovative COF@MXene composites for high performance energy applications

AbstractAs a new type of composite two-dimensional material formed by the combination of Covalent Organic Frameworks (COFs) and two- dimensional (2D) MXenes, COF/MXene heterostructures (COF@MXene) inherit the stable porous two-dimensional structure of COFs and the excellent electrochemical performance and catalytic activity of MXenes, thus attracting widespread attention. Additionally, COF@MXene possesses various elemental affinity sites, efficient ion channels, and the ability to append various functional groups, which endow them with tremendous potential in electrochemical energy storage, energy conversion, and catalysis. Currently, there is a lack of extensive literature discussing the utilization of COF@MXene. The quest for enhanced physicochemical attributes through tailored modifications and composite strategies for COF@MXene is still a noteworthy hurdle. Furthermore, discovering novel application contexts that can harness the exceptional capabilities of these materials presents a formidable task. This review initiates with an exploration of the primary methodologies for synthesizing COF and MXene composites. Subsequently, it outlines the diverse applications of COF and MXene in energy storage, energy conversion, and environmental conservation. Lastly, it discusses the primary obstacles and future trajectories within these domains.

Fluorine-Induced Lattice Oxygen Participation in 2D Layered Double Hydroxide/MXene Hybrids for Efficient Oxygen Evolution.

In oxygen evolution reaction (OER), the participation of lattice oxygen can break the limitation of adsorption evolution mechanism, but the activation of lattice oxygen remains a critical challenge. Herein, a surface fluorinated highly active 2D/2D FeNi layered double hydroxide/MXene (F-LDH/MX) is demonstrated, boosting OER with the enhanced lattice-oxygen-mediated path. The introduction of fluorine promotes the self-evolution of catalyst in an alkaline environment, even without an external current. It further accelerates the formation of active metal oxyhydroxides with abundant oxygen vacancies under the operating potential. The introduced oxygen vacancy activates the lattice oxygen, increasing the proportion of lattice oxygen mechanism in OER. Owing to the synergistic effects of the 2D/2D hierarchical structure and the modulated active surface, F-LDH/MX possesses excellent electrochemical performances, including a low overpotential of 251 mV at 10 mA cm-2, a low Tafel slope of 40.28 mV dec-1, and robust stability. The water electrolyzer system with F-LDH/MX as the anode offers the benchmark current density at a low cell voltage of 1.53 V, while the Zn-air battery with F-LDH/MX as the air electrode exhibits a higher power density of 75.43 mW cm-2. This study presents a promising strategy to design highly active electrocatalysts for energy conversion and storage.

Accelerated Ion-Electron Transport in Bi-Heterostructures Constructed Based on Ohmic Contacts for Efficient Bi-Directional Catalysis of Lithium-Sulfur Batteries.

Although lithium-sulfur batteries have satisfactory theoretical specific capacity and energy density, they are difficult to further commercialize due to the shuttle effect of soluble polysulfides and slow sulfur oxidation kinetics. Based on this, in this work, the catalyst MXene-VS4-SnS2 (MVS), a dual heterostructured catalyst with ohmic contacts, is prepared by a one-step hydrothermal method and electrostatic self-adsorption for lithium-sulfur battery cathode materials. Experimental and theoretical results show that the ohmic contact induces spontaneous charge rearrangement, resulting in the formation of a fast charge transfer pathway at the MVS heterojunction interface, which helps to reduce the energy barrier for polysulfide reduction and Li2S oxidation during the discharge/charge process. In addition, the inherent sulfophilicity of VS4 and SnS2 promotes the conversion of S species, while the pleated MXene nanosheets not only provide a highly conductive network for the active sulfur but also retain a rich internal space to maintain the integrity of the cathode structure during the continuous cycling process. As a result, the MVS cathode exhibits excellent electrochemical performance even under high sulfur loading. The integration of excellent performance with a facile synthesis process provides a promising approach for designing highly efficient electrocatalysts suitable for the energy field.

Preparation and Properties of Fe-Based Double Perovskite Oxide as Cathode Material for Intermediate-Temperature Solid Oxide Fuel Cell

Double perovskite oxides with mixed ionic and electronic conductors (MIECs) have been widely investigated as cathode materials for solid oxide fuel cells (SOFCs). Classical Fe-based double perovskites, due to their inherent low electronic and oxygen ionic conductivity, usually exhibit poor electrocatalytic activity. The existence of various valence states of B-site ions modifies the material’s catalytic activity, indicating the possibility of the partial substitution of Fe by higher-valence ions. LaBaFe2−xMoxO5+δ (x = 0, 0.03, 0.05, 0.07, 0.1, LBFMx) is used as intermediate-temperature solid oxide fuel cell (IT-SOFC) cathode materials. At a doping concentration above 0.1, the Mo substitution enhanced the cell volume, and the lattice expansion caused the formation of the impurity phase, BaMoO4. Compared with the parent material, Mo doping can regulate the oxygen vacancy concentration and accelerate the oxygen reduction reaction process to improve the electrochemical performance, as well as having a suitable coefficient of thermal expansion and excellent electrode stability. LaBaFe1.9Mo0.1O5+δ is a promising cathode material for IT-SOFC, which shows an excellent electrochemical performance, with this being demonstrated by having the lowest polarization resistance value of 0.017 Ω·cm2 at 800 °C, and the peak power density (PPD) of anode-supported single-cell LBFM0.1|CGO|NiO+CGO reaching 599 mW·cm−2.

Understanding of a Ni-Rich O3-Layered Cathode for Sodium-Ion Batteries: Synthesis Mechanism and Al-Gradient Doping.

O3-type NaNi0.8Mn0.1Co0.1O2 (NaNMC811) cathode active materials for sodium-ion batteries (SIBs), with a theoretical high specific capacity (∼187mAhg-1), are in the preliminary exploration stage. This study comprehensively investigates NaNMC811 from multiple perspectives. For the first time, the phase evolution ( - - ) during the solid-state synthesis is systemically investigated, which elucidates in-depth the mechanisms of the thermal sodiation process. Furthermore, an Al-gradient doping of NaNMC811 wassuccessfully implemented through Al2O3 coating on the cathode active material (CAM) precursor. The modified Al-NaNi0.8Mn0.1Co0.1O2 (Al-NaNMC811) exhibits excellent electrochemical dynamics and performance, maintaining a specific capacity above 100mAhg-1 after 100 cycles at 0.1 C (1.5-4.1 V) while providing a promising capacity retention of 63%. Additionally, the material demonstrates excellent rate capabilities, retaining a specific capacity of 107 mAh g-1 at 5 C. Compared to pristine NaNMC811, the modified Al-NaNMC811 is proven to have improved electrochemical kinetics with a higher Na+ diffusion coefficient due to dilated (003) interplanar spacing, and a more stable structure during the electrochemical charge-discharge processes, which is attributed to stronger Al-O bond energy. Understanding phase formations during the synthesis and comprehensive insight in the gradient doping for O3-type NaNMC811 CAMs guides further development of next-generation SIBsmaterials.

N, P co-Doped Hard Carbon Anodes for High-Performance Lithium-Ion Batteries with Enhanced Capacity Retention and Cycle Stability.

Compared to the traditional graphite anode, heteroatom-doped polymer carbon materials have high capacity retention due to their high porosity and porous structure. Therefore, they have great potential for application in lithium-ion battery (LIB) anodes. In this work,an N, P co-doped precursor polymer material (MBPp), synthesized via a one-pot method using bisphenol-A (C-source), melamine (N-source), and 9,10-Dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (P-source). The resulting N, P-co-doped hard carbon materials (MBPs) were prepared at various pyrolysis temperatures, yielding microporous, mesoporous, and macroporous structures. MBP materials demonstrated excellent electrochemical performance as LIB anodes. Notably, MBP-900 achieved a reversible capacity of 262 mAh g-1 at 1000 mA g-1 (in 0.005-2.0 V voltage range) with a capacity retention rate of 97.2% after 1000 cycles. These findings highlight the significance of MBP materials, which possess numerous defects, large layer gaps, and excellent cycle stability, in advancing the development of polymer anode materials for LIBs.

Inorganic‐Organic Composite Cathode Materials for Aqueous Zinc Ion Batteries

AbstractAs potential candidates for large‐scale energy storage systems, aqueous zinc‐ion batteries (AZIBs) have attracted more and more attention from researchers and investors. Tremendous efforts have been devoted to develop high‐efficient cathode materials for improving comprehensive performances of AZIBs. Recently reported inorganic‐organic composite (IOC) cathode materials exhibited excellent electrochemical performance and were generally superior to corresponding inorganic or organic cathode materials. This paper presents a timely review on recent progresses and challenges in IOCs for AZIBs. Preparation strategies of IOCs have been elaborated and categorized, recent advances and main working mechanisms of IOCs are exhibited with a focus on the analysis methods for mechanism studies, outlooks and challenges of IOC cathodes for AZIBs are outlined to guide their future development.

Enhanced electrochemical activity of boron doped cobalt oxide nanoparticles towards supercapacitor application

Doping via metal/nonmetal/metalloid dopants in to the crystal structural surface of cobalt oxide nanoparticles are promising for creating electroactive supercapacitors with excellent electrochemical performance. Herein, we fabricate boron doped cobalt oxide nanoparticles (B@Co3O4) via a facile co-precipitation route for supercapacitor applications. The incorporation of boron into cobalt oxide nanoparticles (3M B@Co3O4) brings a ∼4.2-fold increase in a specific surface area (548.126 m2g-1), decrease in band gap energy and reduced in crystalline size. Consequently, the B doped Co3O4 NPs displays a maximum specific capacitance of 998.12 F/g, which is ∼1.50-fold increased as compared to 668.79 F/g of the pristine Co3O4 NPs at current density 1.5mA/cm2 and scan rate 2mV/s in 1M KOH electrolyte solution. Moreover, 3M B@Co3O4 NPs demonstrates excellent power density 711.14W/kg and high energy density 195.96Wh/kg Wh/kg. Hence, we believe that boron doped cobalt oxide nanoparticles are a promising electroactive material for the supercapacitive applications.

Zinc hexacyanoferrate with open framework for efficient aqueous cobalt ions storage

In this work, we report a high-performance aqueous Co-ion battery with zinc hexacyanoferrate as Co2+ storage material. Owing to the open framework, zinc hexacyanoferrate exhibits excellent electrochemical performance. The reversible capacity of zinc hexacyanoferrate is up to 62.4 mAh g−1 at 5C with ultralow capacity decay (0.0084 % per cycle) within 500 cycles. Even cycled at a higher rate of 10C, zinc hexacyanoferrate still can remain a high capacity retention of 98.8 % after 700 cycles. The excellent electrochemical performance is attributed to the rapid kinetics behavior of Co2+ in the open and stable framework structure. Besides, a joint analysis of in-situ X-ray diffraction, ex-situ Fourier transform infrared spectroscopy and ex-situ X-ray photoelectron spectroscopy verifies the highly reversible structural change of zinc hexacyanoferrate during charge/discharge process. All these evidences suggest that zinc hexacyanoferrate may be a promising host material for Co2+ storage in aqueous rechargeable batteries.

Effect of CNF ratio and pressure on structural and electrochemical performance of hybrid hydrogel for flexible free-standing electrode and sensors

A 2D flexible hydrogel (GO/CNFn) with layered structure and superhydrophilic is synthesized via cross-linking and self-assembling of graphene oxide (GO) with cellulose nanofiber (CNF) through microwave-assisted hydrothermal. CNF acts as “dispersant” and “spacer”, making GO nanosheets uniformly disperse on their surface with less agglomerations. The carboxyl groups and hydrophilicity of CNF effectively improve the charge storage capacity of carbon materials through interactions. When the mass ratio of GO to CNF is 3:1, the GO/CNF1 exhibits an excellent comprehensive electrochemical performance as free-standing electrodes, with the specific capacitance reaching 295 F/g at 0.5 A/g in three-electrode system. The influence of press pressure on GO/CNFn reveals that increasing the pressure improves the hydrophilicity of the electrode, favoring their wettability to aqueous electrolyte. GO/CNF1–6 possesses the highest degree of graphitization, and delivers a highest mass specific capacitance up to 493 F/g at 0.5 A/g. Flexible solid-state symmetric supercapacitor with GO/CNF1–6 as electrodes exhibits an energy density of 20.6 Wh/kg at a power density of 250 W/kg. The good flexibility and biocompatibility of the devices show sensitive current response to biological signals, endowing them potential application prospect in wearable portable electronics and human motion detections.

Nanocubic transition metal sulfides (FeMn)S2@NC synthesised by MOFs facily for supercapacitors

Transition metal sulfides have attracted considerable attention as supercapacitor materials due to their favorable electrochemical properties and low cost. However, challenges such as slow electrochemical kinetics and significant volume changes still persist. In this study, (FeMn)S2@NC nanocubes were synthesized by utilizing MOFs as precursors, employing a solution method to encapsulate Ppy around the periphery, followed by a one-step annealing process. The electrode prepared from (FeMn)S2@NC exhibits a high specific capacitance of 1154 F/g at 1 A/g and retains a specific capacitance of 777 F/g even at a high current density of 5 A/g. After 8000 charge-discharge cycles at 10 A/g, it still maintains a high capacity retention of 94% and close to 100% Coulombic efficiency. The (FeMn)S2@NC//AC capacitor exhibite excellent electrochemical performance with good rate capability and practical value 39.73F/g at 1A/g, 38.26F/g at 2A/g, 26.67F/g at 5A/g, 20.53F/g at 7A/g and 14F/g at 10A/g. Electrochemical testing at 5A/g show 93.3% high capacity retention after 180,000 cycles.

From waste to material strategy: A closed-loop regeneration process of spent LiFePO4 batteries

A closed-loop regeneration route to recover valuable elements from spent LiFePO4 batteries is proposed. After hot-acid leaching, the leaching rates of Li, Fe and P are above 99.8 %, and the graphite powder retain in the residue with grade of 93.33 %. With iron powder cementation, 99.96 % Cu is removed from acid leaching solution to obtain sponge copper. And then 96.67 %Al and 89.30 %F are precipitated in the form of AlPO4(s) and FeF3(s) at pH = 3.75. Li, Fe and P within the purified solution are prepared as LiFePO4 precursors by co-precipitation method, and finally LiFePO4/C materials are synthesized after two-stage calcination. The recycled LiFePO4/C materials demonstrate excellent electrochemical performance with a discharge capacity of 153.1 mAh·g−1 at 0.1C and a capacity retention of 94.0 % after 500 cycles at 1C. The present recycling process provides a strategy for short and efficient regeneration of spent LiFePO4 batteries.

Incorporation of Mo2C nanoparticles to pollen-derived 3D porous carbon as electrocatalyst for high performance lithium-sulfur batteries

The practical application and development of lithium‑sulfur (LiS) batteries are limited by the slow redox reaction kinetics and shuttle effect of polysulfide lithium (LiPSs). To address these issues, three-dimensional porous carbon (PC, derived from rapeseed pollen) modified with molybdenum carbide (Mo2C) nanoparticles is prepared by a simple and environment-friendly method. On the one hand, the PC-Mo2C host material can facilitate the uniform loading of sulfur and reduce its volume expansion due to its porous carbon structure. On the other hand, it mitigates the shuttle effect by effective chemical adsorption of LiPSs to form strong physical confinement and catalyze the conversion of LiPSs via the aid of the decorated Mo2C nanoparticles. Density functional theoretical calculations also illustrate the Mo2C nanoparticles are capable of inhibiting the shuttle of LiPSs and further improving the cycling stability. The results show that the PC-Mo2C/S electrode exhibits excellent electrochemical performance with high cycle stability (fading rate of 0.066 % per cycle at 0.2C and 0.054 % per cycle at 1C) and outstanding rate capacity (623.2 mAh g−1 at 5C).

Nano ZnO modified amorphous carbon materials enabling long-cycle performance and high-capacity for lithium/sodium-ion batteries

Zinc-modified carbon materials exhibit high specific capacity, good safety, and low self-discharge, making them promising anode materials for lithium-ion and sodium-ion batteries. However, the high cost of raw materials, complex fabrication processes, and limited cycle life remain significant challenges to their further development. In this study, we elucidated a two-step process, simple in technique and suitable for large-scale production, for in-situ zinc modification of amorphous carbon. The synthesized carbon material exhibited superior reversible specific capacity (maintaining 780.27 mAh·g−1 capacity after 80 cycles at 50 mA·g−1 current density), high cycling stability (maintaining Coulombic efficiency at 100.06 % after 15,000 cycles at 10 A·g−1 current density), and good application value (achieving a capacity of 89.67 mAh·g−1 after 1000 cycles at 200 mA·g−1 current density for the assembled MFAC-Zn||NVP full cell). Through our investigation, we discovered that Nano ZnO not only directly participate in electrochemical reactions but also effectively improve the microstructure of amorphous carbon, increasing its three-dimensional axial stacking and providing more reaction sites. The enrichment of open pores significantly enhances the diffusion efficiency of ions within the carbon-based matrix. The superior diffusion ability of alkali metal-ion in the electrode is the reason for the excellent electrochemical performance of Zinc-modified amorphous carbon. Moreover, the incorporation of Nano ZnO aids in the formation of a robust and thin SEI layer. This significantly enhances the stability of the electrode materials during cycling and improves charge transfer efficiency during the charge-discharge process. Our study provides a new strategy for adjusting the internal microstructure of amorphous carbon materials to achieve high-performance lithium/sodium storage.

Naturally superionic polymer electrolyte of macromolecular lignin for all-solid-state sodium-ion batteries at room temperature

Solid polymer electrolytes (SPEs) that offer superior safety, mechanical strength and flexibility are crucial for advancing next-generation sodium-ion batteries (SIBs). Conventional SPEs often display temperature sensitivity, leading to relatively low ionic conductivity at room temperature (RT). Herein, lignin-based SPEs (LG-SPEs) are created by solvation and desolvation of lignin and sodium bis(fluorosulfonyl)imide (NaFSI). Theoretical calculations reveal that lignin (containing rich functional groups) and FSI− molecules facilitate the movement of Na-ions within the electrolyte by minimizing steric hindrance and offering migration sites. Consequently, LG-SPEs demonstrate an enhanced ionic conductivity of 3.4 × 10−4 S cm−1 at RT, with a Na-ion transfer number as high as 0.53. The assembled all-solid-state SIB comprising Na3V2(PO4)3/LG-SPE/NaTi2(PO4)3 exhibits excellent electrochemical performance at RT, achieving a specific capacity of 95 mA h g−1 and retaining 82% of its capacity after 200 cycles at 0.1 C. This work presents an environmentally friendly and straightforward methodology for developing high-performance SPEs at RT, while also opening up new avenues for the valorization of lignin.

Mitigating Long Range Jahn‐Teller Ordering to Stabilize Mn Redox Reaction in Biphasic Layered Sodium Oxide

AbstractTo develop the next‐generation commercial oxide cathodes for sodium‐ion batteries, it is crucial to reduce the expensive Ni element content, and further regulate redox reaction of cheap transition metal elements such as Mn to elevate specific capacity. Nevertheless, the activation of Mn redox reaction (MRR) remains a challenge, and notably, MRR induces pronounced Jahn‐Teller effect, resulting in severe structural distortion and fast performance decay. Herein, activated by Na vacancies and weakened hybridization of O (2p)‐TM (3d‐t2g) orbital, a biphasic low‐Ni Mn‐based oxide P2/O3‐Na0.8Ni0.23Fe0.34Mn0.43O2 (P2/O3) exhibits reversible MRR, which performs the transition between Mn4+ and Mn3+ during charging and discharging. Due to the interlaced arrangement of P2‐type and O3‐type crystal domains in P2/O3, the long range Jahn‐Teller ordering is restricted to mitigate the cooperative distortion of MnO6 octahedron induced by MRR and the Jahn‐Teller effect is suppressed, ensuring sustained stable involvement of MRR in charge compensation. In addition, owing to the introduction of P2‐type phase, there is a significant reduction of the migration barrier for sodium ions and no obvious capacity decline after air exposure, leading to a marked enhancement in dynamic performance and air stability of P2/O3, respectively. Consequently, P2/O3 exhibits excellent electrochemical and processing performance.

Unravelling the electrochemical characteristics and sodium storage mechanism of pistachio shell derived hard carbon as high plateau capacity anodes by operando Raman spectroscopy and full cell demonstration

Hard carbon has emerged as a highly promising material for negative electrode in sodium-ion batteries (SIBs). This study focuses on the synthesis of an anode material through the pyrolysis of Pistachio shells, a commonly available nut waste, at different temperatures ranging from 900° to 1400°C. The material pyrolyzed at 1400 °C exhibits a remarkable reversible discharge capacity of 302 mAhg−1 and plateau capacity of 223 mAhg−1 at a current rate of 10 mAg−1, displaying stable cyclic performance and an impressive 80% capacity retention after 500 cycles at 200 mAg−1. The morphological, structural, and surface chemical characteristics of the cycled hard carbon anode materials were examined through ex-situ FE-SEM, XRD, and XPS analyses. Furthermore, the sodiation and desodiation mechanisms of the synthesized hard carbon were investigated using operando Raman Spectroscopy. The diffusion kinetics parameters were determined by Electrochemical Impedance Spectroscopy (EIS) and CV analyses. This study underscores the potential of Pistachio shells as a promising precursor for the synthesis of carbonaceous anode for SIBs, employing a straightforward one-step pyrolysis process. The excellent electrochemical performance, along with the ease of material sourcing and synthesis, places this nutty waste as a promising, sustainable and clean energy resource option for advancing sodium-ion battery technology.

Hierarchical Flower Array NiCoOOH@CoLa‐LDH Nanosheets for High‐Performance Supercapacitor and Alkaline Zn Battery

AbstractNickel oxyhydroxide based energy storage materials have been largely confined by insufficient exposure of active sites which results in low energy efficiency and poor stability. In order to resolve the problems, hierarchical flower array heterostructure NiCoOOH@CoLa‐LDH (denoted as NC@CL) nanosheets are designed with NiCo oxyhydroxide (NiCoOOH, denoted as NC) being tightly covered on CoLa layered double hydroxide (CoLa‐LDH, denoted as CL) nanosheet. This rational design creates more active sites, enlarges the electrode‐electrolyte contact area, improves electron conductivity, and prevents agglomeration during the cycling charge–discharge processes. Density functional theory calculations and differential charges concurrently illustrate that heterostructure formation optimizes the reaction kinetics and promotes electron redistribution. Benefiting from the heterogeneous structure and rich electro‐active sites caused by NC, NC@CL displays outstanding reversible specific capacitance (3228 F g−1 at 1 A g−1). The aqueous rechargeable alkaline Zn battery NC@CL//Zn exhibits a high capacity of 381.1 mA h g−1 at 0.5 A g−1 and cycling durability (98% capacity retention after cycling at 5 A g−1 for 2000 cycles). The excellent electrochemical performances indicate that NC@CL has great application potential as electrode material for aqueous energy storage device.