Stable Anode Research Articles

Coupling Solvation Structure Regulation and Interface Engineering via Reverse Micelle Strategy Toward Highly Stable Zn Metal Anode

AbstractThe stability of aqueous Z inc (Zn) ion energy storage devices is significantly compromised by the instability at the electrode/electrolyte interface, which can result in the growth of Zn dendrites, self‐corrosion, and various other side reactions. Regulating the Zn‐ion （Zn2+) solvation structure through electrolyte additives has been proved to be effective strategy in stabilizing the Zn anode, but the influence of free water on the solvation structure is often lacking in‐depth exploration. Herein, the piperazine‐N,N‐bis(2‐hydroxypropanesulfonic acid) sodium salt (POPSO‐Na) is presented as a multifunctional electrolyte additive, which enhances the stability of the Zn anode by modulating the deposition and stripping environment of Zn2⁺ and limiting the presence of free water in the electrolyte during cycling. Theoretical calculation and experimental results demonstrate that the POPSO‐Na additive can not only replace the structural water around Zn2+ to destroy the original solvation sheath, but also form reverse micelle interface structure to hinder the proton transition and constrain the free water in the electrolyte. Thus, the Zn||Zn battery utilizing the ZnSO4+POPSO‐Na electrolyte exhibits an impressive cycle life of 1600 h at a current density of 1 mA cm−2, achieving an average Coulomb efficiency (CE) of ≈100%, which is significantly better than that observed with the ZnSO4 electrolyte. Moreover, the Zn||Cu battery with ZnSO4+POPSO‐Na electrolyte achieves high stability even after cycling for over 2000 h.

Crystallographic Reorientation Induced by Gradient Solid-Electrolyte Interphase for Highly Stable Zinc Anode.

Oriented zinc (Zn) electrodeposition is critical for the long-term performance of aqueous Zn metal batteries. However, the intricate interfacial reactions between the Zn anode and electrolytes hinder a comprehensive understanding of Zn metal deposition. Here, the reaction pathways of Zn deposition and report the preferential formation of Zn single-crystalline nuclei followed by dense Zn(002) deposition is elucidated, which is induced by a gradient solid-electrolyte interphase (SEI). The gradient SEI composed of abundant B-O and C species facilitates faster Zn2+ nucleation rate and smaller nucleus size, promoting the formation of Zn single-crystalline nuclei. Additionally, the homogeneity and mechanical stability of SEI ensure the crystallographic reorientation of Zn anodes from Zn(101) to (002) planes, efficiently inhibiting dendrite growth and metal corrosion during the Zn2+ stripping/plating process. These advantages significantly enhance the stability of the Zn anode, as demonstrated by the prolonged cycling lifespan of symmetric Zn batteries and exceptional reversibility (>99.5%) over 5000 cycles in Zn//Cu asymmetric batteries. Notably, this strategy also enables the stable operation of anode-free Zn//I2 batteries with a long lifespan of 3000 cycles. This work advances the understanding of Zn electrochemical behaviors, encompassing Zn nucleation, growth, and Zn2+ stripping/plating.

Organic-Inorganic Hybrid Solid Composite Electrolytes for High Energy Density Lithium Batteries: Combining Manufacturability, Conductivity, and Stability.

The deployment of solid and quasi-solid electrolytes in lithium metal batteries is envisioned to push their energy densities to even higher levels, in addition to providing enhanced safety. This article discusses a set of hybrid solid composite electrolytes which combine functional properties with electrode compatibility and manufacturability. Their anodic stability >5V versus Li+/Li and compatibility with lithium metal stem from the incorporated ionic liquid electrolyte, whereas the organic-inorganic hybrid host structure boosts their conductivity up to 2.7mScm-1 at room temperature. The absence of strong acids enables compatibility with porous NMC811 electrodes. Liquid precursor solutions can be readily impregnated into porous electrodes, facilitating cell assembly. Electrolytes containing TFSI- as the only anion have a superior compatibility toward high-voltage positive electrode materials, whereas electrolytes containing both FSI- and TFSI- have a better compatibility toward lithium metal. Using the former as catholyte and the latter as anolyte, NMC811/Li coin cells retain up to 100% of their initial capacity after 100 cycles (0.2C, 3.0-4.4V vs Li+/Li). Because of their unprecedented combination of functional properties, electrode compatibility, and manufacturability, these hybrid solid composite electrolytes are potential candidates for the further development of lithium metal battery technology.

ZnO Quantum Dots as PEO-Based Solid Electrolytes Fillers for Lithium Metal Batteries.

PEO-based solid polymer electrolyte (PEO SPE) is regarded as one of the most promising solid electrolytes due to its exceptional flexibility, cost-effectiveness, and ease of integration. However, its commercialization is hindered by inadequate ionic conductivity and unstable interface. By incorporating proper ZnO quantum-dots (QDs) fillers with enhanced surface activity, the ion transport inner the PEO-based electrolyte can be improved along with enhanced REDOX kinetics at the Li/PEO interface. The ionic conductivity reaches 5.97×10-4 S cm-1 at 60 °C. Moreover, ZnO QDs exhibit a quantum size effect and possess lithiophilic characteristics that promote uniform nucleation and redeposition of Li+ while forming a stable Li-Zn alloy. This inhibits lithium dendrite formation and enhances the stability of Li anode. Li//Li cell with 3 % ZnO QDs works steadily for more than 2100 h at 60 °C with 0.1 mA cm-2. The assembled Li//LiFePO4 cell provides a reversible capacity of 134.91 mAh g-1 after200 cycles at 0.1 C.

Concurrent Regulation of Surface Topography and Interfacial Physicochemistry via Trace Chelation Acid Additives toward Durable Zn Anodes

AbstractElectrolyte additive engineering is a feasible protocol in improving Zn anode stability. Typical additive designs center on the regulation of Zn deposition; nevertheless, versatile additives are urgently requested to comprehensively manage the surface landscape, interface physicochemistry, and by‐product elimination. Here, a straightforward strategy is presented to meet such needs employing an environmentally‐friendly chelator, hydroxyethyl‐ethylenediaminetriacetate acid (HEDTA), as an additive for ZnSO4 electrolyte. Throughout theoretical computations and experimental investigations, it is demonstrated that protons released from the gradual ionization of HEDTA during rest periods aid in the mild engraving of the Zn surface. Both the amino and carboxyl groups of HEDTA⁻ can be protonated, which effectively buffers the interfacial pH value in the entire battery lifespan and eliminates the formation of by‐products. The HEDTA− anions can also adsorb onto the Zn surface, helping facilitate Zn2⁺ mass transfer and accelerate the desolvation process. Benefiting from the synchronous modulation of surface topography and interfacial physicochemistry, the assembled half cells affording HEDTA additive maintain a durable operation of up to 8821 cycles at 5.0 mA cm−2/1.0 mAh cm−2. Additionally, symmetric cells manifest stable cycling for over 4600 h at 0.5 mA cm−2/0.25 mAh cm−2.

Polyethylene Glycol-Protected Zinc Microwall Arrays for Stable Zinc Anodes.

Aqueous zinc-ion batteries promise good commercial application prospects due to their environmental benignity and easy assembly under atmospheric conditions, positioning them as a viable alternative to lithium-ion batteries. However, some inherent issues, such as chaotic zinc dendrite growth and inevitable side reactions, challenge the commercialization progress. In this work, we imprint highly ordered zinc microwall arrays to regulate the electric field toward uniform Zn deposition. Afterward, coating a polyethylene glycol protection layer on the zinc microwalls aims to passivate the surface defects that rise unintentionally by mechanical imprinting. Polyethylene glycol can also boost oriented Zn deposition along the (002) plane and inhibit hydrogen gas production, further enhancing the stability of such three-dimensional (3D) hybrid anodes. Compared to the messy electric field near the polyethylene glycol-protected Zn foil, the uniform electric field provided by these 3D hybrid anodes can regulate the Zn deposition behaviors, enabling a longer lifespan and thus certifying the necessity of adding 3D microstructures. Additionally, 3D microstructures can offer a larger surface area than that of the planar Zn foil, providing more reaction sites and higher specific capacity. In this case, the 3D hybrid electrode exhibits a good initial capacity of approximately 120 mA h/g at a current density of 5 A/g and a nice retention of more than 80% after 800 cycles. The proposed scheme paves the way for a long-term stable 3D zinc anode solution with promising application prospects.

Oriented and Continuous Phase Epitaxy Enabled by A Highly Dendrite‐Resistant Plane Toward Super‐High Areal Capacity Zinc Metal Batteries

AbstractUnstable Zn metal anodes with dendrites/side reactions are becoming the main obstacle to the practical application of zinc‐based aqueous batteries. Epitaxial growth has been considered to be an effective strategy for solving these issues, especially for inducing the (002) plane growth. Nonetheless, the (002)‐textured Zn is difficult to achieve highly stable Zn anode under high capacity resulting from its large lattice distortion. Herein, the Cu single atom anchored polymeric carbon nitride (Cu@PCN) is synthesized by a facile thermal polymerization method. Serving as multifunctional protective layer on Zn surface, the Cu@PCN can provide massive nucleation sites at a nano‐level and uniformize the electron distribution through coordination engineering. Optimizing the coordination structures of single Cu and N atoms within the carbon matrix enables a redistribution for electric field and regulates ion flux. More importantly, this coordination strategy with single atoms is first reported to customize oriented and continuous phase epitaxy along highly dendrite‐resistant Zn(101) plane by reducing (101) surface energy. This pattern of oriented dense deposition leads to stable and reversible Zn plating/stripping is achieved, which delivers an extended cycling life of 550 h at 10 A cm−2, 20 mAh cm−2. The practical full cell also displays stable performance for 1200 cycles.

Formicarium-Like Micron Porous Si Synergistically Adjusted by Surface Hard-Soft Nanoencapsulation as Long-Life Lithium-Ion Battery Anode.

Micron porous silicon (MPSi) is a promising lithium-ion battery (LIB) anode that can provide enough space to effectively alleviate the volume expansion and large number of transmission channels to rapidly transport the Li-ions. However, a long-term stable MPSi anode at high current density is still a great challenge. Herein, a double-regulated formicarium like-MPSi composite using the surface hard-soft titanium dioxide-few layered MXene nanotemplate (FMPSi@TiO2@FMXene) was designed and synthesized via an in situ assembly strategy as long-life LIB anode. Such hard-soft TiO2-FMXene nanoencapsulation can collaboratively tune the internal/external stress, inhibit the volume expansion, reduce the interfacial reactions, and improve the electrical conductivity of MPSi, resulting in the great enhancement of structural stability and electrochemical performance in cycling even at high current density. Especially, this FMPSi@TiO2@FMXene anode exhibits a high reversible capacity of 1254.9 and 970.4 mAh/g after 500 cycles at 0.5 and 1 A/g, respectively. Moreover, a full cell is assembled with the FMPSi@TiO2@FMXene anode and commercial LiFePO4 (LFP) cathode, exhibiting a high capacity retention rate of 91.6% in 100 cycles. This work provides an effective surface nanoengineering tactic to obtain the structurally stable MPSi anodes by hard-soft nanotemplate for large-scale and long-term LIB application.

Sulfurized Composite Interphase Enables a Highly Reversible Zn Anode.

The stability and reversibility of Zn anode can be greatly improved by in-situ construction of solid electrolyte interphase (SEI) on Zn surface via a low-cost design strategy of ZnSO4 electrolyte. However, the role of hydrogen bond acceptor -SO3 accompanying ZnS formation during SEI reconstruction is overlooked. In this work, we have explored and revealed the new role of -SO3 and ZnS in the in-situ formed sulfide composite SEI (SCSEI) on Zn anode electrochemistry in ZnSO4 aqueous electrolytes. Structure characterization and DFT demonstrate that the introduction of -SO3 can not only reduce the dehydration energy of [Zn(H2O)6]2+, but also enhance the stability of the ZnS/Zn interface and homogenize the ZnS/Zn interface electric field, thereby significantly improving the dynamic kinetics and uniform deposition of Zn2+. Owing to the synergistic effect of ZnS and -SO3, a high cycling stability of 1500 h with a cumulative-plated capacity of 7.5 Ah cm-2 at 10 mA cm-2 has been achieved within the symmetrical cell. Furthermore, the full cell with NH4V4O10 cathode exhibits outstanding cyclic stability, exceeding 2000 cycles at 5 A g-1 and maintaining a Coulombic efficiency of 100%. These new insights into anionic synergistic strategy could significantly enhance the practical application of zinc-ion batteries.

Sulfurized Composite Interphase Enables a Highly Reversible Zn Anode

The stability and reversibility of Zn anode can be greatly improved by in‐situ construction of solid electrolyte interphase (SEI) on Zn surface via a low‐cost design strategy of ZnSO4 electrolyte. However, the role of hydrogen bond acceptor ‐SO3 accompanying ZnS formation during SEI reconstruction is overlooked. In this work, we have explored and revealed the new role of ‐SO3 and ZnS in the in‐situ formed sulfide composite SEI (SCSEI) on Zn anode electrochemistry in ZnSO4 aqueous electrolytes. Structure characterization and DFT demonstrate that the introduction of ‐SO3 can not only reduce the dehydration energy of [Zn(H2O)6]2+, but also enhance the stability of the ZnS/Zn interface and homogenize the ZnS/Zn interface electric field, thereby significantly improving the dynamic kinetics and uniform deposition of Zn2+. Owing to the synergistic effect of ZnS and ‐SO3, a high cycling stability of 1500 h with a cumulative‐plated capacity of 7.5 Ah cm‐2 at 10 mA cm‐2 has been achieved within the symmetrical cell. Furthermore, the full cell with NH4V4O10 cathode exhibits outstanding cyclic stability, exceeding 2000 cycles at 5 A g‐1 and maintaining a Coulombic efficiency of 100%. These new insights into anionic synergistic strategy could significantly enhance the practical application of zinc‐ion batteries.

3D-stacked electrospun iron-doped nickel cobalt oxide nanofibers as integrated electrodes for anion exchange membrane water electrolysis

The commercialization of anion-exchange membrane water electrolysis (AEMWE) requires the development of highly active, stable, and cheap anode catalysts for the oxygen evolution reaction (OER). In this study, we proposed electrospun iron-doped NiCo2O4 (NCO) nanofibers on nickel foam (NF) and evaluated the performances of the resulting samples (FeX-NCO/NF; X = iron loading in NCO (0, 5, 10, and 15 at %)) as unitized anodes for the OER. Among the fabricated electrodes, Fe10-NCO/NF exhibited the lowest overpotential of 352 mV at a current density of 50 mA cm−2 in a half-cell test owing to its improved intrinsic activity. In an AEMWE single-cell test, Fe10-NCO/NF as anode showed high current density (932 mA cm-2 at 1.8 V) and long-term stability for 150 h The improved AEMWE performance of Fe10-NCO/NF was attributed to efficient mass transport enabled by superhydrophilic three-dimensional porous structure featuring stacked nanofibers.

Biomineralization Inspired the Construction of Dense Spherical Stacks for Dendrite-Free Zinc Anodes.

Aqueous zinc-ion batteries (AZIBs) are considered to be one of the most promising energy storage systems due to their high degree of safety and low cost. However, the deposition of the uncontrolled zinc dendritic morphology on the surface of the Zn anode seriously reduces the cycle life of AZIBs. Herein, inspired by natural biomineralization, a uniform spherical zinc deposition is achieved via the addition of a biological macromolecule to the electrolyte. The proposed biological macromolecule makes Zn2+ undergo dense spherical deposition by regulating the relative growth rate of high-index planes of metal zinc, effectively avoiding the destruction from irregular zinc dendrites. The symmetric cell with the addition of such a biological macromolecule can be stably cycled for >3200 h at 1 mA cm-2 for 1 mAh cm-2. This work sheds light on expanding morphological regulation of metal deposition to spherical shapes for stable metal anodes in addition to a single-crystal plane control strategy.

Sn Penetrated Zincophilic Interface Design in Porous Zn Substrate for High Performance Zn-Ion Battery.

Rechargeable zinc-ion batteries are considered an ideal energy storage system due to their low cost and nonflammable aqueous electrolyte. However, dendrite growth, hydrogen evolution reaction, and self-corrosion of zinc anode brought about serious safety risks including short circuits and electrode expansion. Therefore, a modified host-design strategy with a 3D porous structure and bulk-phase penetrated zincophilic interface is proposed to boost the stability and lifetime of the Zn anode. The porous Zn substrate is constructed by universal HCl etching and the uniform and tight Sn-penetrated zincophilic interface is formed by effective electron beam evaporation (EBE). The porous substrate can uniform zinc ion flux and the Sn coating could effectively improve zinc ion deposition behavior, thus inhibiting the risk of dendrites growth and side reaction. As a result, the 3D Zn substrate with Sn interface (3D Zn@Sn) exhibits prolonged galvanostatic cycling performance up to 4500h with a low polarization of ≈25mV (1mAcm-2, 1mAhcm-2) in the symmetric cell. The full cell assembled with KVOH@Ti could maintain a high specific capacity of 148.6mAhg-1 after 500 galvanostatic cycles (10Ag-1). This work proposed an improved electrode design to realize the high performance of zinc ion batteries.

Porous V2CTx MXene as a High Stability Zinc Anode Protective Coating.

Aqueous Zn batteries exhibit significant research potential owing to their environmental friendliness and high energy density. Nevertheless, the formation of dendrites on the zinc anode and the sluggish diffusion kinetics of zinc ions adversely affect the cycle life of zinc ion batteries. In this study, we employ porous V2CTx (MVMX) as a protective layer for the zinc anode. The uniform porous structure of MVMX promotes active site exposure and facilitates the transport of zinc ions. Remarkably, the Zn@Ti half-cell demonstrated an average CE of 99.7% in 1500 cycles. Furthermore, the Zn-Zn symmetric battery exhibited stable cycling for 1600 h at current densities of 5 mA cm-2 and 1 mAh cm-2. Additionally, the MVMX@Zn||V2O5 full cell exhibited a capacity of 198 mAh g-1 and retained a capacity of 124.75 mAh g-1 after 5000 cycles at 1 A g-1, demonstrating the potential of employing alternative MXenes for fabricating stable zinc anodes.

Molecular Chain Rearrangement of Natural Cellulose‐based Artificial Interphase for Ultra‐stable Zn Metal Anodes

The unstable electrolyte‐anode interface, plagued by parasitic side reactions and uncontrollable dendrite growth, severely hampers the practical implementation of aqueous zinc‐ion batteries. To address these challenges, we developed a regenerated cellulose‐based artificial interphase with synergistically optimized structure and surface chemistry on the Zn anode (RC@Zn), using a facile molecular chain rearrangement strategy. This RC interphase features a drastically increased amorphous region and more exposed active hydroxyl groups, facilitating rapid Zn2+ diffusion and homogeneous Zn2+ interface distribution, thereby enabling dendrite‐free Zn deposition. Additionally, the compact texture and abundant negatively charged surface of the RC interphase effectively shield water molecules and harmful anions, completely preventing H2 evolution and Zn corrosion. The superior mechanical strength and adhesion of the RC interphase also accommodate the substantial volume changes of Zn anodes even under deep cycling conditions. Consequently, the RC@Zn electrode demonstrates an outstanding cycling lifespan of over 8000 hours at a high current density of 10 mA cm‐2. Significantly, the electrode maintains stable cycling even at a 90% depth of discharge and ensures stable operation of full cells with a low negative/positive capacity ratio of 1.6. This study provides new solution to construct highly stable and deep cycling Zn metal anodes through interface engineering.

Molecular Chain Rearrangement of Natural Cellulose-based Artificial Interphase for Ultra-stable Zn Metal Anodes.

The unstable electrolyte-anode interface, plagued by parasitic side reactions and uncontrollable dendrite growth, severely hampers the practical implementation of aqueous zinc-ion batteries. To address these challenges, we developed a regenerated cellulose-based artificial interphase with synergistically optimized structure and surface chemistry on the Zn anode (RC@Zn), using a facile molecular chain rearrangement strategy. This RC interphase features a drastically increased amorphous region and more exposed active hydroxyl groups, facilitating rapid Zn2+ diffusionand homogeneous Zn2+ interface distribution, thereby enabling dendrite-free Zn deposition. Additionally, the compact texture and abundant negatively charged surface of the RC interphase effectively shield water molecules and harmful anions, completely preventing H2 evolution and Zn corrosion. The superior mechanical strength and adhesion of the RC interphase also accommodate the substantial volume changes of Zn anodes even under deep cycling conditions. Consequently,the RC@Zn electrode demonstrates an outstanding cycling lifespan of over 8000 hours at a high current density of 10 mA cm-2. Significantly, the electrode maintains stable cycling even at a 90% depth of discharge and ensures stable operation of full cells with a low negative/positive capacity ratio of 1.6. This study provides new solution to construct highly stable and deep cycling Zn metal anodes through interface engineering.

Triple-Layered Noncombustible PEO-Based Solid Electrolyte for Highly Safe Lithium-Metal Batteries.

Lithium-metal batteries are currently recognized as promising next-generation technologies owing to their high energy density. Solid polymer electrolytes, particularly those based on polyethylene oxide (PEO), are lauded for their leakage resistance, safety, and flexible design. Despite the ongoing fire safety- and ionic conductivity-related concerns, a novel noncombustible solid polymer electrolytes with superior ionic conductivities are introduced here with additive decabromodiphenyl ethane and zeolite. To enhance the mechanical strength and ensure soft interactions at the electrode interface, a triple-layer structure with self-extinguishing properties and robust ionic conductivity is proposed. Notably, the softness at the electrode interface intensifies as the LiTFSI concentration increases; this higher concentration negatively impacts PEO crystallinity, enhancing the ionic conductivity owing to the presence of free Li+ and TFSI- ions. This novel electrolyte can achieve a conductivity of 1.5 mS cm-1 at 60°C, maintain anodic stability up to 4.8V, and exhibit flame retardancy. Furthermore, adding LiTFSI at 60% relative to PEO is shown to reduce LiF formation on the surface, enhancing anode stability. The [LiFePO4/triple-layered electrolyte/Li] lithium-metal batteries are capable of an initial capacity of 153 mAh g-1, sustained superior capacity retention of 87.9%, and high Coulombic efficiency (99.6%) over 1000 cycles at a 1C rate.

Achieving stable lithium metal anode via constructing lithiophilicity gradient and regulating Li3N-rich SEI

Three-dimensional (3D) current collectors are studied for the application of Li metal anodes in high-energy battery systems. However, they still suffer from the preferential accumulation of Li on the outermost surface, resulting from an inadequate regulation of the Li+ transport. Herein, we propose a deposition regulation strategy involving the creation of a 3D lithiophilicity gradient structure of MoN on Cu3N nanowire-grown Cu foam (MCNCF) to induce a “bottom-up” Li deposition. During the initial Li deposition, the reaction between Li and Cu3N leads to the formation of Li3N while the lithiophilic MoN located at the bottom promotes the downward Li+ migration, resulting in the generation of a Li3N gradient. Such a “bottom-up” Li3N distribution results in the formation of a stable and Li3N-rich solid electrolyte interphase layer, facilitating the Li⁺ transport and promoting a uniform Li nucleation. Computational simulations and experimental results corroborate the preferential deposition of Li on the bottom of the substrate, leading to a uniform Li nucleation and growth throughout the electrode. The MCNCF electrode offers a significantly improved reversibility of the Li deposition, achieving a lifespan of more than 1200 h at a current density of 1 mA cm−2 in symmetric Li||Li cells. Furthermore, full-cells incorporating MCNCF@Li as the negative electrode and LiFePO4 cathodes exhibit outstanding electrochemical performance with a capacity retention of over 99.5 % after 250 cycles at 1 C, which significantly surpasses the performance achieved with CF@Li or CCF@Li electrodes. This innovative design strategy for 3D metallic current collectors, featuring a lithiophilicity gradient, provides new perspectives for the development of stable Li metal anodes and, as a result, for the advancement of Li-metal batteries.

Rational design of alginate-derived network binder for high-performance silicon-based anodes in Li-ion batteries

This study developed a novel alginate-derived network binder, SAH, to enhance the performance and stability of silicon-based anodes in lithium-ion batteries. Integrating acrylic acid and 2-hydroxyethyl acrylate with sodium alginate through a one-pot polymerization and in-situ cross-linking method, SAH effectively addresses the volumetric expansion challenges associated with silicon anodes. This innovative binder maintains the structural integrity of the silicon anode through its rigid acrylic acid component, while the flexible acrylic-2-hydroxyethyl ester serves as a dynamic buffer to enhance flexibility. Sodium alginate contributes its intrinsic beneficial properties and imparts a robust three-dimensional network structure through effective coupling, allowing the binder to accommodate silicon volume changes during battery operation. Consequently, lithium-ion batteries incorporating this binder exhibited improved stability and extended cycle life, achieving an impressive capacity retention rate of 87.3 % after 100 cycles at 0.5C. This study highlights the potential of biopolymeric materials in enhancing the functionality of silicon-based anodes, contributing to the ongoing development of high-performance energy storage technologies.

Nanofluid channels mitigated Zn2+ concentration polarization prolonged over 30 times lifespan for reversible zinc anodes

Despite interfacial engineering protects zinc anode from electrolyte corrosion, the suppressed kinetics process on the anode surface/interface circumscribes their cyclic stability, especially dendritic growth induced by ion concentration gradients. Here, the zinophilic nanofluid channels (ZNC) protective layer on zinc surface are designed for the rapid Zn2+ transport kinetic in the reversible cycling process. The ZNC demonstrates high separation pressure between ions and the channel surface due to the capillary effect, allowing Zn2+ to quickly migrate along the channel wall (Zn2+ transference numbers up to 0.72). Therefore, the unique channel modules alleviate concentration polarization from rapid Zn2+ consumption and maintain uniform deposition of Zn ions. Consequently, The ZNC protective layer anode exhibits significantly improved cycle life by more than 30 times (over 4000 h at 1 mA cm−2) that of bare Zn. The full battery exhibits stable cycling performance with excellent capacity retention (∼100%) after 5000 cycles. Our work provides innovative insights into the role of nanofluids in improving the stability of zinc anodes, offering enlightening perspectives for long-cycle life zinc-based batteries.