Layered Double Hydroxide Nanosheets Research Articles

Utilizing cationic vacancies to enhance nickel-cobalt layered double hydroxides for efficient electrocatalytic urea oxidation reaction

Electrocatalytic urea oxidation reaction (UOR) is a promising approach for urea-rich wastewater splitting, which benefits for reducing energy consumption in hydrogen production accompanying environmental protection and sustainable energy development. To address the limitations posed by the self-oxidation of nickel-based catalysts on the activity of UOR, we here developed a NiCo LDH nanosheet catalyst with abundant Ni vacancies to initiate the UOR process prior to nickel oxidation. Electrochemical impedance spectroscopy and In-situ spectroscopic characterizations confirm that the UOR process primarily occurs on the surface of the catalyst, rather than being driven by nickel oxidation products. The favorable electronic structure modulation induced by Ni vacancies makes the catalyst more energetically favorable for the UOR compared to nickel self-oxidation. The catalyst exhibits excellent UOR activity, only requiring 1.27 V vs. RHE at 10 mA cm−2 and 1.34 V vs. RHE at 100 mA cm−2, with no significant decay observed after over 120 h of operation. Furthermore, it can function as a bifunctional catalyst, requiring only 1.66 V to achieve 100 mA cm−2 for the UOR||HER system. This study expands the pathway for the application of cationic vacancies in UOR.

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.

Construction of a hydrophobicity, phosphorus‐ and nitrogen‐containing layered double hydroxides‐based synergistic effect flame retardant for poly (lactic acid)

AbstractIn this work, a synergistic effect strategy was explored for fabricating hydrophobicity, phosphorus‐ and nitrogen‐containing layered double hydroxides nanosheets (LDHs) based flame retardant (LDHs‐K@DM). This fabricating process was achieved by amination of the surface of LDHs and, subsequently, interfacial self‐assembly with high P content of diethylenetriaminpenta (methylene‐phosphonic acid) (DTPMP) and high N content of melamine (MEL). The chemical construction and thermal stabilization properties of LDHs‐K@DM were confirmed via different characterization approaches. The results revealed that LDHs‐K@DM was successfully prepared and the surface of LDHs‐K@DM was transformed into hydrophobicity with high water contact angle. Moreover, LDHs‐K@DM had better thermal stability. After that, LDHs‐K@DM was molten compounded with biobased polylactic acid (PLA). It was suggested that LDHs‐K@DM were uniformly dispersed in the PLA matrix and could accelerate the decomposition of PLA to form char residues. Most importantly, the addition of 20 wt% LDHs‐K@DM into PLA can endow the composite to achieve a desirable UL‐94 V‐0 rating and the limiting oxygen index value of 30.9%. Finally, the synergistic effect flame retardant mechanism of LDHs‐K@DM was comprehensively analyzed. This synergistic decorating strategy for preparing LDHs‐K@DM flame retardant is promising for industrial production.

Carboxymethyl cellulose based edible nanocomposite coating with tunable functionalities and the application on the preservation of postharvest Satsuma mandarin fruit

This study introduces an innovative carboxymethyl cellulose (CMC)-based edible nanocomposite coating, with two-dimensional layered double hydroxide nanosheets (2D LDH-NSs) and shellac, engineered to address challenges in fruit preservation. The synergistic integration of shellac and LDH-NS into the CMC matrix is strategically designed with tunable functionalities, encompassing wettability, gas barrier, and tensile properties. Our findings reveal that incorporating shellac and LDH-NS significantly improves the coating's wettability on the mandarin fruit surface, thus bolstering its adherence and uniformity, alongside enhancing its water vapor barrier efficacy and influencing the oxygen permeability. The application of this novel edible nanocomposite coating on Satsuma mandarin (Citrus unshiu Marc.) fruits has yielded promising outcomes in prolonging postharvest shelf life while preserving essential quality attributes, including peel surface morphology, weight loss, hardness, color retention, and nutritional values. Our work signifies a significant leap forward for the edible coating technology and bolsters the postharvest preservation of perishable fruits.

PAD4 Inhibitor-Loaded Layered Double Hydroxide Nanosheets as a Multifunctional Nanoplatform for Photodynamic Therapy-Mediated Tumor Metastasis Treatment.

Photodynamic therapy (PDT) is demonstrated to be effective in inducing antitumor immune responses for tumor metastasis treatment. However, tumor hypoxia, inferior tissue penetration of light, and low singlet oxygen (1O2) quantum yield significantly hamper the efficacy of PDT, thus weakening its immune function. Moreover, PDT-mediated neutrophil extracellular traps (NETs) formation can further reduce the therapeutic effectiveness. Herein, the use of defect-rich CoMo-layered double hydroxide (DR-CoMo-LDH) nanosheets as a carrier to load a typical peptidyl arginine deiminase 4 inhibitor, i.e., YW4-03, to construct a multifunctional nanoagent (403@DR-LDH) for PDT/immunotherapy, is reported. Specifically, 403@DR-LDH inherits excellent 1O2 generation activity under 1550nm laser irradiation and improves the half-life of YW4-03. Meanwhile, 403@DR-LDH plus 1550nm laser irradiation can stimulate immunogenic cell death to promote the maturation of dendric cells and activation/infiltration of T cells and significantly downregulate H3cit protein expression to inhibit NETs formation, synergistically promoting the antitumor metastasis effect. Taken together, 403@DR-LDH can kill cancer cells and inhibit tumor growth/metastasis under 1550nm laser irradiation. Single-cell analysis indicates that 403@DR-LDH can regulate the ratio of immune cells and immune-related proteins to improve the tumor immune microenvironment, showing strong efficacy to inhibit the tumor growth, metastasis, and recurrence.

Interface-engineered Ni(Fe/Al)-LDHs/g-C3N4 nanosheets with metallic Fe/Al[sbnd]N bonds for efficient photocatalytic degradation of tetracycline hydrochloride

To improve the photogenerated electron–hole separation efficiency and the number of reactive oxygen species of g-C3N4 in visible light. Herein, an interface-engineered Ni(Fe/Al)-LDHs/g-C3N4 nanosheets with Fe/AlN bonds were prepared, which shows highly enhanced photocatalytic degradation performance with excellent structural stability. The interfacial structure of g-C3N4 was precisely regulated by metal Fe/Al on the surface of layered double hydroxides (LDHs), which could form Fe/AlN bonds as the interfacial charge transfer channels. In addition, the metal Ni and Fe/Al on the surface of LDHs nanosheets can furnish more photocatalytic active sites and interface synergy. The obtained 7 %NiFe-LDHs/g-C3N4 owns the degradation rate of 99.23 % for tetracycline hydrochloride (TCH) in visible light. This work highlights a rational interface engineering strategy for the formation of a composite structure with interface interaction for efficient photocatalysts.

Hydroxy salt induced CoAl-LDH nanosheet composite membrane for pervaporation desalination

Pervaporation is a promising desalination technology. Developing high-performance and stable pervaporation membranes with high continuity structure remains a significant challenge. This study reports the development of a novel layered double hydroxide (LDH) nanosheet composite membrane fabricated using a hydroxyl salt induction method. This approach facilitated the in-situ nucleation and growth of the CoAl-LDH nanosheets on polyvinylidene fluoride (PVDF) substrate, reducing precursor concentration and enhancing preparation efficiency. The resulting cross-compatible architecture closely integrated the dense LDH nanosheet separation layer with the flexible PVDF support. The microstructure and morphology of the hydroxyl salt layer and its transformed CoAl-LDH composite membrane were comprehensively investigated. The optimized membrane was applied for pervaporation desalination (3 wt% NaCl, 50 °C), achieving a high flux of 38.4 kg·m−2·h−1 and exceptional NaCl rejection of 99.9 %. It also demonstrated excellent tolerance to a wide salinity range, maintaining 99.6–99.9 % rejection even at 20 wt% NaCl, while the flux remained stable at 26.7 kg·m−2·h−1. Long-term testing confirmed the consistent separation performance and operational stability, underscoring the great potential of this advanced membrane material for practical pervaporation desalination applications.

Synergistic adsorption-photocatalytic remediation of methylene blue dye from textile industry wastewater over NiFe LDH supported on tyre-ash derived activated carbon

The photocatalytic performance of the multilayered NiFe LDH/Activated Carbon was evaluated for the degradation of methylene blue (MB) in industrial textile wastewater, considering prior adsorption on the photocatalyst surface. The XRD, XPS, BET, TEM and FE-SEM results confirmed that the highly exposed mesoporous layers, carbon backbone, and interlayer anions serve as active sites responsible for the adsorption of MB dye due to the expected electrostatic interactions. Electrochemical methods such as CV, LSV and EIS revealed the improved conductivity and supported the interactions observed. Encouraged by these interactions, the irradiation of visible light enabled the degradation of methylene blue, and the degradation products were monitored using UPLC chromatograms and MS spectra. The removal efficiencies of the MB dye were found to be 17.5 %, 51.2 %, 67.1 %, 84.8 %, and 94.2 % due to photolysis, adsorption, and degradation on AC, NiFe LDH nanosheets, and NiFe LDH/AC nanocomposite, respectively. The results of the UPLC chromatograms and MS spectra suggested that MB was mineralized into simpler fragments after 30 min of visible light irradiation. Scavenging studies were examined using a series of scavenging agents. However, the maximum photodegradation was attained in the absence of the scavengers. The reusability studies showed that the MB photodegradation efficiency declined by 20.8 %, possibly due to the loss of the catalyst during the washing step. Nonetheless, the NiFe LDH/AC structure remained intact, suggesting the strong stability of the photocatalyst. The plausible degradation mechanism and probable degradation pathway of MB were outlined and supported by the chromatographs and MS results. The overall results suggest that photocatalysis of cationic dyes such as MB on NiFe LDH/AC should be encouraged to work towards sustainable solutions for textile water treatment.

Determination of methotrexate using carbon paste electrode modified with ionic liquid/Ni-Co layered double hydroxide nanosheets as a voltammetric sensor.

Methotrexate (MTX) is a widely used anti-cancer drug, but its overuse can lead to significant side effects. Therefore, it is very vital to design simple and sensitive analytical methods for its determination. In this work, an electrochemical sensor was prepared based on an ionic liquid (IL)/Ni-Co layered double hydroxide nanosheets (Ni-Co-LDH)-modified carbon paste electrode IL/Ni-Co-LDH/CPE. Cyclic voltammetry, differential pulse voltammetry, and chronoamperometry methods were applied to evaluate the performance of the designed sensor for MTX determination. The IL/Ni-Co-LDH/CPE sensor exhibits a linear relationship between the peak current of the differential pulse voltammetry and MTX concentrations in the linear dynamic range of 0.02 to 140.0 μM, with a detection limit of 0.006 μM. The IL/Ni-Co-LDH/CPE sensor exhibited relative standard deviation values between 1.7 to 3.7 % for recovery tests on real samples, indicating the precision of the method. The designed sensor with cost-effective and good performance could be valuable for therapeutic drug monitoring and clinical diagnostics.

Exploration of adsorption properties of organic corrosion inhibitors on layered double hydroxide nanosheet: A molecular dynamics simulation study

Understanding the adsorption of organic corrosion inhibitors with different functional groups on layered double hydroxide (LDH) nanosheet is crucial for the synthesis of these protective materials. In this study, the adsorption process of five deprotonated organic corrosion inhibitors—lactate (Lc), 2-hydroxybenzothiazole (2-OH-BTH), 2-mercaptoethanesulfonic acid (MS), N,N-dimethylethanolamine (DMEA), and eugenol (EG)—on LDH nanosheets was simulated. The adsorption rate, adsorption configuration, and adsorption stability between LDH nanosheet and organic corrosion inhibitors were investigated throughout the entire adsorption process. The study observed consistency in the adsorption rate and stability of these organic corrosion inhibitors in the following order: Lc > 2-OH-BTH > MS > DMEA > EG. Additionally, hydrogen bonds between the organic corrosion inhibitors and the LDH nanosheet is the primary mechanism driving adsorption. The number and stability of hydrogen bonds influenced both the adsorption rate and stability. It is noteworthy that 2-OH-BTH and DMEA have not previously been incorporated into LDH. There is potential for these two organic corrosion inhibitors to be modified for LDH, suggesting significant prospects for future research.

N/O-bridge stimulated robust binding energy and fast charge transfer between carbon nanofiber and NiCo LDH for advanced supercapacitors

Layered double hydroxide (LDH)-carbon composites effectively mitigate the inherent issues of agglomeration and poor conductivity in LDH. However, the weak binding energy and insufficient charge transfer capability between LDH and carbon substrate significantly compromise the active substance loading, cyclic stability and practical capacity of the composites. Herein, N/O co-doping porous carbon nanofibers (NOPCNFs) are first prepared by blending diminutive zinc imidazolate framework-8 nanoparticles with polyacrylonitrile for electrospinning, and then densely packed NiCo LDH nanosheets are homogeneously anchored on NOPCNFs to form NiCo LDH@NOPCNFs heterostructure via a hydrothermal method. The experimental findings and density functional theory calculation results indicate that N/O atoms exhibit robust binding forces with metal atoms through enhanced electrostatic adsorption and p-d covalent hybridization, which facilitates the nucleation and development of NiCo LDH on carbon nanofibers. Meanwhile, these heteroatoms also serve as the bridge for electron transfer from NiCo LDH to NOPCNF, leading to a strong interfacial electric field, thus accelerating charge transfer behaviors. Benefitting from the synergistic interaction between NiCo LDH and NOPCNF, the obtained NiCo LDH@NOPCNFs demonstrate an elevated mass loading of active substance (55 wt%), an impressive specific capacitance of 1340 F/g at 1 A/g (based on the mass of NiCo LDH, 2463 F/g), and good cyclic durability for 5000 cycles. Moreover, an all-solid-state asymmetric supercapacitor using NOPCNFs and NiCo LDH@NOPCNFs shows promising practical application prospects. This work gives insights into the important influence of heteroatom doping in carbon, and provides a feasible approach for the efficient integration of electroactive and carbon material.

Tunable Growth of Layered Double Hydroxide Nanosheets through Hydrothermal Conversion of Atomic Layer Deposition Seed Layers

Tunable Growth of Layered Double Hydroxide Nanosheets through Hydrothermal Conversion of Atomic Layer Deposition Seed Layers

Microplasma-assisted construction of cross-linked network hierarchical structure of NiMoO4 nanorods @NiCo-LDH nanosheets for electrochemical sensing of non-enzymatic H2O2 in food

The accumulation of small doses of hydrogen peroxide (H2O2) into food can cause many diseases in the human body, and it is urgent to develop efficient detection methods of H2O2. Herein, the hierarchical structure composite of NiCo-LDH nanosheets crosslinked NiMoO4 nanorods was grown in situ on carbon cloth (NiMoO4 NRs@NiCo-LDH NSs/CC) by micro-plasma assisted hydrothermal method. Thanks to the synergistic effect of three metals and (NiMoO4 NRs@NiCo-LDH NSs/CC) provided by nanorods/nanosheets hierarchical structure, NiMoO4 NRs@NiCo-LDH NSs/CC exposes more active sites and achieves rapid electron transfer. The H2O2 electrochemical sensor was constructed as the working electrode with a linear range of 1 μmol L−1 to 9.0 mmol L−1 and detection limit of 112 nmol L−1. In addition, the sensor has been successfully applied to the detection of H2O2 in food samples, the recovery rate is 95.2%–106.62%, RSD < 4.89%.

Piezoelectric Bilayer Nickel-Iron Layered Double Hydroxide Nanosheets with Tumor Microenvironment Responsiveness for Intensive Piezocatalytic Therapy.

Piezocatalytic therapy (PCT) based on 2D layered materials has emerged as a promising non-invasive tumor treatment modality, offering superior advantages. However, a systematic investigation of PCT, particularly the mechanisms underlying the reactive oxygen species (ROS) generation by 2D nanomaterials, is still in its infancy. Here, for the first time, biodegradable piezoelectric 2D bilayer nickel-iron layered double hydroxide (NiFe-LDH) nanosheets (thickness of ≈1.86nm) are reported for enhanced PCT and ferroptosis. Under ultrasound irradiation, the piezoelectric semiconducting NiFe-LDH exhibits a remarkable ability to generate superoxide anion radicals, due to the formation of a built-in electric field that facilitates the separation of electrons and holes. Notably, the significant excitonic effect in the ultrathin NiFe-LDH system enables long-lived excited triplet excitons (lifetime of ≈5.04µs) to effectively convert triplet O2 molecules into singlet oxygen. Moreover, NiFe-LDH exhibited tumor microenvironment (TME)-responsive peroxidase (POD)-like and glutathione (GSH)-depleting capabilities, further enhancing oxidative stress in tumor cells and inducing ferroptosis. To the best of knowledge, this is the first report on piezoelectric semiconducting sonosensitizers based on LDHs for PCT and ferroptosis, providing a comprehensive understanding of the piezocatalysis mechanism and valuable references for the application of LDHs and other 2D materials in cancer therapy.

Hierarchical triplet-metallic oxide/carbon nanocomposites constructed from 2D layered double hydroxides and metal-organic frameworks for high-performance microwave absorption

In the face of increasingly severe electromagnetic wave radiation and interference, it is of great significance to design and prepare excellent absorbing materials. Particularly, hierarchical structure has emerged with enhanced physicochemical properties, offering enormous potential for designing absorbing materials. Here, a hierarchical structure composite constructed by ZIF-8 and fungus-like nickel-cobalt layered double hydroxide (Ni, Co-LDH) nanosheets were synthesized by in-situ self-assembly growth process. A series of Zn@NiCo-Lc composites were obtained by calcination under air. Calcined derivatives of dielectric and magnetic metallic oxides and carbon give rise to multiple polarizations and magnetic losses. The matching of the dielectric and magnetic losses of the hybrid material is further tuned by varying the feed ratio of the bimetallic LDH nanosheets, resulting in a sample with tunable EMA performance. All samples exhibit comparable EMA performance, especially large EABmax of above 5.5 GHz, and Zn@NiCo-Lc-2 has the strongest EMA intensity performance (RLmin is −67.61 dB at an ultra-thin thickness of 1.71 mm). This study provides a tractable method for the fabrication of hierarchical structural composites of high-performance MOF/LDH-derived absorbers, further broadening the application and development of novel electromagnetic wave absorption materials.

Flexo-Phototronic Boosted Self-Powered Ultraviolet Detection in ZnAl:Layered Double Hydroxide Nanosheets/NiO Heterostructure.

Developing self-powered and flexible optoelectronic sensors with high responsivity and speed is crucial for modern applications, motivating continuous efforts to enhance their performance. Flexo-phototronics is a less-explored but promising technique to elevate the performance of optoelectronics. Therefore, this work addresses the potential of utilizing the flexo-phototronic effect to enhance the performance of a flexible and self-powered ultraviolet photodetector (UV PD) based on ZnAl:LDH (layered double hydroxides) nanosheets (Ns)/NiO heterostructure. The vertically oriented ZnAl:LDH Ns are synthesized via a simple method involving the immersion of a sputtered 10% Al-doped ZnO thin film in deionized water at room ambient conditions. The fabricated PD exhibits an impressive response to 365 nm UV light, with high sensitivity in the order of 103. The device's photocurrent and responsivity are significantly enhanced by the flexo-phototronic effect, attributed to the flexoelectric properties of ZnAl:LDH Ns. Specifically, applying an inhomogeneous tensile strain of 2% boosted the device responsivity by 57.1% and improved its operational speed. Furthermore, a working model revealing the altered energy-band structure is demonstrated to elucidate the flexo-phototronic-induced boost in the photoresponse. The PD also demonstrated a sustainable performance under severe bending cycles, underlining the good flexibility of the device. The results presented in this study demonstrate a self-powered and flexible UV PD and provide a viable approach to augment the performance of optoelectronics through the flexo-phototronic effect.

One-step exfoliation and etching of layered double hydroxide nanosheets to construct nanofiltration membranes with high water permeance

Two-dimensional nanosheets are considered promising materials for membranes. However, the excessively long interlayer channels parallel to the membrane surface are not conducive to molecular transport. Creating defects on the nanosheets is an effective method to shorten the transport distance in the membrane. This study involved exfoliating and etching several commonly used layered double hydroxide (LDH) nanosheets using an alkali solution in a single step. This process resulted in porous oligolayered nanosheets modified layered double hydroxide (MgAl-MLDH) with an average pore size of approximately 18 ± 2 nm and a thickness of around 8 nm. These ultrathin porous MgAl-MLDH nanosheets were used to create a composite membrane using a vacuum-assisted filtration method. The structure of the MgAl-MLDH membrane was optimized by adjusting the etching conditions. The water flux of MgAl-MLDH membrane in Eriochrome black T aqueous solution was 530 L/m2 h MPa. Compared with the non-etched LDH membrane (179 L/m2 h MPa), the permeance of MLDH membrane was increased by 2 to 3 times, while the rejection rate remained at approximately 99 %. Furthermore, due to the excellent strength of LDH, the membrane exhibited good stability in both structure and separation performance.

Interlayer-spacing regulation of NiFe LDH nanosheets cathode with high rate performance for chloride ion battery

Chloride ion batteries (CIBs) possess the multiple advantages of high theoretical volumetric energy density, abundant precursor resources and high safety due to the dendrit-free characteristic, which provide more choices and opportunities for electrochemical energy storage. In this work, NiFe LDH nanosheets with different interlayer spacing are prepared using a simple co-precipitation method with the interlayer spacing of LDH nanosheets extended from 7.695 Å to 24.114 Å. Expanding interlayer space of LDHs nanoplates helps to the promote ion diffusion and enhance their action kinetics. Additionally, the increased oleophobicity between NiFe LDH nanosheets cathode with increased interlayer spacing and solvent PC is beneficial for the structural stability of the materials during cycling. Compared with typical chloride ion-intercalated NiFe LDH nanosheets, the NiFe-C17H25O3 LDH with the maximum interlayer spacing demonstrates a performance improvement of about 213 % (with a discharge specific capacity of 64.2 mAh/g after 200 cycles) at high current density and good rate performance. This work provides a simple and effective interlayer spacing control strategy for the design of CIBs cathodes under high current density.

Tuning built-in potential of NiP/NiFe LDH p-n junction towards efficient electrocatalytic water and urea oxidation

Oxygen evolution reaction (OER) and urea oxidation reaction (UOR) are critical half-reactions to realize sustainable hydrogen production. However, the sluggish dynamics derived from the multi-electron pathways necessitate the exploration for efficient catalysts. Herein, a p-n junction nanorod array composed of Mo doped NiP nanorod and ultrathin NiFe LDH nanosheets (NiMoP/NiFe LDH) is proposed to regulate charge distribution of interface for triggering decomposition of water and urea. The p-n junction with a powerful built-in potential (EBI) of 1.2 V at the interface facilitates the adsorption and fracture of chemical group in water and urea molecules. Consequently, the heterostructured electrode demonstrates exceptional electrochemical performance with ultralow potentials of 1.43 and 1.33 V (vs. RHE) at 10 mA cm−2 for OER and UOR, respectively. The overall urea electrolysis driven by NiMoP/NiFe LDH needs only 1.51 V to deliver 100 mA cm−2. This work demonstrates a promising strategy to regulate the EBI of semiconductor heterostructure for energy conversion and sewage treatment.

Construction of an anti-anionic-depletion layer to mitigate the tip deposition effect for dendrite-free zinc anode

Rechargeable aqueous zinc-ion batteries have been plagued by the well-known problem of zinc dendrite formation. This issue mainly arises from the inherent depletion of anions in the vicinity of the zinc anode during deposition process, leading to a strong spatial electric field that influences Zn2+ cations deposition and triggers dendrite growth. Herein, the anti-anionic-depletion strategy is proposed that involves anions anchored in the surface region of zinc anode to mitigate the adverse effects of the spatial electric field and inhibit dendrite growth. By theoretical calculations and experimental verification, layered double hydroxides (LDHs) materials were selected to immobilize SO42- anions and construct a protective coating layer against anion depletion (anti-anionic-depletion layer). Furthermore, the deposition flux of Zn2+ cations was also regulated by in-situ growing LDH nanosheets. Benefiting from these modifications, the in-situ grown ZnAl-LDH modified electrode (Zn@ZnAl) exhibits outstanding stability (5500 cycles at 40 mA cm−2), and shows negligible capacity degradation in both Zn-Mn full cells and zinc hybrid capacitors.