Rechargeable aqueous zinc-ion batteries (AZIBs) are regarded as a promising large-scale energy storage technology due to their inherent safety, cost-effectiveness, and environmental friendliness^[1-4]. However, their practical application is largely limited by the interfacial instability of the zinc anode^[5,6]. Compared to zinc foil, which is commonly used in basic research, zinc powder anodes offer a higher specific surface area and are favored by industry for scalable electrode fabrication^[7]. Yet, this high surface area exacerbates parasitic reactions such as hydrogen evolution and corrosion during cycling. Moreover, the substantial volume changes of zinc particles easily lead to fragmentation, loss of electrical contact, accumulation of “dead zinc”, and rapid coulombic efficiency decay^[8-11]. Therefore, stabilizing the interface of zinc powder anodes has become a critical challenge for the commercialization of AZIBs.

The failure of zinc powder anodes essentially stems from uncontrolled ion transport and deposition behavior at the electrode-electrolyte interface^[12,13]. An ideal interface layer should not merely serve as a physical barrier but should actively regulate Zn²⁺ flux and deposition kinetics. Various strategies have been explored, including the construction of conductive frameworks, crystal orientation regulation^[14-16], and electrolyte engineering^[17,18]. However, most of them rely on prefabricated static structures. Such “pre-set” protective layers often fail in dynamically evolving local environments during electrochemical cycling, particularly under severe volume fluctuations at high areal capacity. Cracking, delamination, and eventual loss of protection are common.

In response to these limitations, recent efforts have focused on in situ formation of stable interfacial phases^[19,20]. Although in situ-formed solid electrolyte interphase (SEI)-like films can passivate the surface to some extent, maintaining stable and effective interfacial regulation over extended cycling remains challenging^[21-23]. The key scientific challenge is thus overcoming the “rigidity” of the interfacial chemistry to shift from “passive protection” to “active regulation” that evolves synergistically with electrochemical processes.

Here, we propose an interface regulation strategy based on copper oxalate (CuC₂O₄) embedded directly into the zinc powder electrode matrix, rather than being introduced as an electrolyte additive. Unlike conventional in situ SEI formation^[19,20], CuC₂O₄ is not a static coating but a functional component that undergoes a discharge-triggered phase transition. The phase transformation refers to the electrochemically driven conversion of crystalline Cu(II)-oxalate into a structurally disordered, C-O-enriched and Cu⁺-containing interphase, rather than a conventional crystallographic phase transition between two well-defined crystalline phases. During cathodic polarization, the Cu(II)-oxalate framework becomes destabilized in the hydrated electrochemical environment, leading to a coupled evolution of the carbon-oxygen coordination environment (from C=O-rich to C-O-enriched) and reduction of Cu²⁺ to Cu⁺. Consequently, the interface dynamically reconstructs into a new phase rich in C-O groups and Cu⁺-related active sites, which modulates Zn²⁺ adsorption/desolvation and suppresses competitive water reduction. As a result, the CuC₂O₄-modified zinc powder anode (ZP@CuC₂O₄) exhibits significantly enhanced cycling stability. In Zn||Zn symmetric cells, it operates stably for approximately 600 h at 7 mA cm^-2/1 mAh cm^-2 and shows a substantial lifespan extension over unmodified controls at 10 mA cm^-2/1 mAh cm^-2. In Zn||V₂O₅ full cells, ZP@CuC₂O₄ retains a capacity of 78 mAh g^-1 after 3,600 cycles at 10 A g^-1 at 25 °C. At 40 °C, it maintains approximately 118 mAh g^-1 after 800 cycles at 10 A g^-1. Moreover, pouch-type full cells deliver a cumulative capacity of 11.7 Ah after 1,000 cycles at 7 A g^-1. This work demonstrates that intrinsic, phase-transition-driven interfacial coordination reconstruction can transform a zinc powder anode from a passively protected electrode to an actively regulating system, offering a new paradigm for durable aqueous zinc batteries.

Figure 1 schematically illustrates the proposed interfacial regulation mechanism based on CuC₂O₄. In the pristine zinc powder electrode, the particle-packed structure creates spatially dispersed active sites and pronounced local polarization, leading to preferential Zn²⁺ desolvation and nucleation at limited sites, which causes high nucleation overpotential, dendritic growth, and hydrogen evolution^[24-27]. In contrast, CuC₂O₄ does not act as a static coating. Instead, it is proposed to undergo a discharge-induced structural and coordination reconstruction at the electrode/electrolyte interface. During cathodic polarization, the original Cu(II)-oxalate units gradually destabilize and evolve toward Cu(I)-related species, while the local carbon-oxygen coordination environment shifts from a C=O-rich state to a more C-O-enriched configuration^[28]. This phase transition is attributed to continuous electron injection combined with the interfacial instability of the initial Cu(II)-oxalate framework in the hydrated electrochemical environment, inducing coupled Cu-valence reduction and ligand bonding reorganization. This interpretation is consistent with prior reports on electron-induced oxalate removal/decomposition from Cu(II) oxalate and the conversion-type phase evolution of transition-metal oxalates under electrochemical reduction^[28-30]. The resulting interfacial coordination reconstruction generates more uniformly distributed Zn-O interaction sites, enhances local zincophilicity, and simultaneously modulates the interfacial behavior of Zn²⁺ and H₂O. Consequently, Zn²⁺ adsorption and desolvation become more spatially homogeneous, interfacial energy fluctuation and polarization accumulation are alleviated, and the interface selectivity for Zn deposition over parasitic reactions is improved^[31,32]. As a result, zinc deposition becomes more uniform and reversible, with suppressed dendritic growth and hydrogen evolution.

To identify the appropriate CuC₂O₄ loading, electrodes containing 1, 2, 5, and 8 wt% CuC₂O₄ were first evaluated in Zn//Zn symmetric cells under different current densities and areal capacities. As shown in Supplementary Figures 1-3 [Supplementary Materials], the electrode containing 2 wt% CuC₂O₄ consistently exhibited the longest lifetime under 0.5 mA cm^-2/0.25 mAh cm^-2, 5 mA cm^-2/1 mAh cm^-2, and 7 mA cm^-2/1 mAh cm^-2. These results indicate that an appropriate CuC₂O₄ content is important for optimizing the electrochemical performance of the Zn powder electrode. The inferior cycling performance at lower CuC₂O₄ contents may reflect insufficient interfacial regulation, whereas the deterioration at higher contents could qualitatively arise from an increased inactive fraction and potentially less favorable electronic/ionic transport within the electrode. However, because systematic impedance or conductivity measurements were not performed for electrodes with different CuC₂O₄ loadings, the latter interpretation remains a qualitative conjecture rather than a quantitatively verified mechanism. Based on the cycling-performance optimization, 2 wt% CuC₂O₄ was therefore selected for subsequent mechanistic and electrochemical investigations, and the corresponding electrode was designated as ZP@CuC₂O₄.

The optimized ZP@CuC₂O₄ electrode exhibits significantly enhanced rate capability and cycling durability compared to the pristine ZP electrode. Under increasing current densities, ZP@CuC₂O₄ maintains reduced voltage hysteresis and stable plating/stripping behavior [Figure 2A]. Specifically, the cycle life extends from 160 h to 650 h at 0.5 mA cm^-2 [Supplementary Figure 4, Supplementary Materials] and from 192 h to 700 h at 1 mA cm^-2 /1 mAh cm^-2 [Figure 2B]. Robust stability is further demonstrated at higher current densities, with stable cycling achieved for 520 h at 5 mA cm^-2 [Supplementary Figure 5, Supplementary Materials], approximately 600 h at 7 mA cm^-2/1 mAh cm^-2 [Figure 2C], and approximately 370 h under the rigorous condition of 10 mA cm^-2/1 mAh cm^-2, where the control electrode failed prematurely [Figure 2D]. High zinc utilization and lean-Zn operation are important considerations for evaluating the practical viability of Zn-metal batteries^[33]. To further evaluate the deep-discharge tolerance of the Zn powder anode, the areal capacity was increased to 2 mAh cm^-2 at 7 mA cm^-2. Under this more demanding condition, ZP@CuC₂O₄ maintained a more stable voltage response with suppressed polarization growth compared with pristine ZP during repeated Zn plating/stripping [Supplementary Figure 6, Supplementary Materials]. Moreover, the interfacial regulation strategy proves effective at elevated temperatures. At 40 °C, ZP@CuC₂O₄ delivers a stable voltage profile, in contrast to the rapid deterioration of the bare electrode [Figure 2E]. The superior performance of this strategy is highlighted in comparison with previously reported zinc-based electrodes [Figure 2F and Supplementary Table 1, Supplementary Materials]. Consistent trends were observed in Zn//Cu cells. At 0.2 mA cm^-2/0.1 mAh cm^-2, ZP@CuC₂O₄ sustained 575 cycles with an average coulombic efficiency (CE) of 98.1%, whereas the ZP electrode failed after 187 cycles [Figure 2G]. At 1 mA cm^-2/0.5 mAh cm^-2, the pristine electrode failed after only 166 cycles with an average CE of 98.63%, while ZP@CuC₂O₄ maintained a high CE of 99.55% for more than 420 cycles [Figure 2H]. These results demonstrate that CuC₂O₄ substantially enhances the reversibility and long-term electrochemical stability of the zinc powder anode.

Electrochemical kinetics and interfacial stability were further examined to clarify how CuC₂O₄ improves the zinc powder anode. The Tafel plots show that ZP@CuC₂O₄ exhibits a lower corrosion current and a more positive corrosion potential than the pristine ZP electrode [Figure 3A], indicating improved corrosion resistance^[34]. This protective effect is further corroborated by LSV [Figure 3B], where the ZP@CuC₂O₄ electrode exhibits a reduced cathodic current in the negative potential region compared with the pristine ZP electrode, indicating a suppressed hydrogen evolution reaction^[35]. Regarding the deposition kinetics, the nucleation overpotential in Zn//Cu cells decreases from 21.7 to 17.3 mV upon modification [Figure 3C]. This reduction indicates that the CuC₂O₄ modification lowers the Gibbs free energy barrier for zinc nucleation, thereby promoting homogeneous nucleation and mitigating dendrite growth^[31,32]. In situ electrochemical impedance spectroscopy coupled with distribution of relaxation times (DRT) analysis was employed to monitor the time-dependent interfacial kinetics during Zn plating/stripping [Figure 3D and E]. The short-, intermediate-, and long-relaxation-time regions [log₁₀(τ/s) ≈ -5 to -3, -3 to -1, and -1 to 1] are qualitatively associated with fast interfacial/surface-film processes, charge-transfer processes, and slower ion-transport/concentration-polarization processes, respectively. During plating, pristine ZP shows progressively intensified intermediate- and long-time responses, followed by a broad increase after polarity reversal at ~3,600 s, whereas ZP@CuC₂O₄ shows weaker, more localized DRT features, indicating reduced impedance accumulation and more stable interfacial kinetics during repeated plating/stripping.

To corroborate the electrochemical findings, SEM and EDS mapping were employed to visualize the morphological evolution and elemental distribution of the electrodes. Prior to cycling, SEM images and corresponding EDS mapping confirm the homogeneous incorporation of Cu-containing species within the ZP@CuC₂O₄ architecture [Supplementary Figures 7 and 8, Supplementary Materials], establishing a uniform initial interface. Following 100 cycles at a current density of 1 mA cm^-2, the unmodified ZP electrode exhibits severe morphological degradation. The surface is characterized by rough, loose accumulations and distinct localized protrusions [Figure 3F], indicative of uncontrolled dendritic growth and uneven zinc deposition. Concurrently, elemental mapping reveals a complete absence of copper signals [Figure 3G-I], confirming the lack of a protective modulator layer. In stark contrast, the cycled ZP@CuC₂O₄ electrode maintains a planar, compact, and dendrite-free morphology [Figure 3J]. The corresponding elemental maps [Figure 3K-M] display a highly uniform distribution of Cu, O, and Zn across the electrode surface. This persistent uniformity suggests that the CuC₂O₄ modification possesses robust structural integrity, rather than detaching or deactivating during prolonged cycling. The interfacial layer continues to effectively regulate ion flux and guide the homogeneous expansion of the reaction zone, thereby preventing the formation of “dead zinc” and ensuring stable plating/stripping behavior. Cross-sectional SEM further shows a more heterogeneous and discontinuous through-thickness morphology for the cycled ZP electrode, whereas ZP@CuC₂O₄ retains a comparatively more continuous and uniform internal structure [Supplementary Figure 9, Supplementary Materials]. Such suppression of localized Zn growth is consistent with previous interfacial-regulation studies demonstrating that homogenized interfacial Zn²⁺ transport and deposition can mitigate dendritic growth and parasitic reactions^[36]. To further evaluate the morphological stability of the Zn anode under elevated-temperature conditions, post-cycling SEM and EDS characterizations were performed on electrodes retrieved from Zn//Zn symmetric cells cycled at 40 °C. Compared with pristine ZP, ZP@CuC₂O₄ retains a more compact, uniform surface morphology and a more homogeneous elemental distribution after high-temperature cycling [Supplementary Figure 10, Supplementary Materials].

To elucidate how CuC₂O₄ regulates the zinc anode interface during operation, multimodal spectroscopic characterizations were performed on ZP@CuC₂O₄ before and after discharge. The structural origin of the introduced modifier was first verified using CuC₂O₄ powder. Its XRD pattern matches the reported CuC₂O₄ phase well, with a characteristic (110) reflection near 22.7°, confirming the crystallographic identity of the modifier [Supplementary Figure 11, Supplementary Materials]^[37]. Raman spectroscopy also shows characteristic vibrational features associated with coordinated oxalate species, indicating that the initial CuC₂O₄ phase contains a distinct carbonyl-dominated coordination environment [Supplementary Figure 12, Supplementary Materials]^[38]. After discharge to -1.2 V, however, the characteristic (110) diffraction peak of CuC₂O₄ disappeared [Figure 4A], indicating that the original crystal structure had been disrupted. This structural evolution was further corroborated by vibrational spectroscopy. In the FT-IR spectrum, the ν(C=O) vibration was markedly weakened, whereas the ν(C-O) vibration was significantly enhanced, accompanied by an intensified ν(-OH) signal [Figure 4B]. It should be noted that the ν(-OH) band is not sufficiently specific for an unambiguous structural assignment and may also contain contributions from adsorbed/interfacial water, residual electrolyte, and hydroxide- or basic zinc salt-related species formed during cycling. Therefore, the ν(-OH) variation is considered only as auxiliary evidence, while the proposed reconstruction is primarily supported by the coordinated changes in the C=O/C-O features together with the XRD and XPS results. Raman results likewise show that the characteristic C=O peak near 1,520 cm^-1 became markedly weaker after discharge [Figure 4C]. These results consistently indicate that CuC₂O₄ did not remain structurally unchanged during discharge, but instead underwent a discharge-triggered phase transition, in which the original Cu(II)-oxalate framework evolved from a C=O-dominated state toward a more C-O-enriched configuration.

XPS results provide more direct chemical evidence for this phase transition. In the O 1s spectrum, the pristine electrode surface was primarily characterized by Zn-O species from the native oxide layer, together with distinct C=O and C-O components arising from the oxalate coordination structure of CuC₂O₄. After discharge, the Zn-O peak was markedly weakened, whereas the C-O-related component was significantly enhanced, indicating that the interfacial oxygen environment shifted from an initial Zn-O/C=O-rich state toward a more C-O-enriched configuration [Figure 4D]. Consistently, the O-C=O signal in the C 1s spectrum decreased, while the C-O component increased simultaneously [Figure 4E], suggesting that the original Cu-oxalate coordination environment was partially transformed from a carbonyl-dominated state into a more C-O-enriched single-bond configuration during discharge^[28]. Further evidence was provided by the Cu 2p spectrum. Cu in the pristine electrode mainly existed as Cu²⁺, whereas after discharge the main peaks shifted to lower binding energies and the satellite peaks largely disappeared, indicating the formation of Cu⁺-related species [Figure 4F]^[28]. A plausible explanation is that cathodic electron injection destabilized the Cu(II)-oxalate framework in the hydrated interfacial environment, thereby inducing reduction of the Cu center together with reorganization of oxalate ligand bonding^[28,29,39]. These results collectively demonstrate the first key mechanistic feature: the discharge-triggered phase transition of CuC₂O₄ itself. While the present characterization primarily captures the structural and chemical states before and after discharge, future operando spectroscopic studies could provide further insight into the temporal evolution and reversibility of the interfacial reconstruction. Complementary in-situ electrochemical techniques, such as scanning electrochemical microscopy (SECM), may further provide spatially resolved information on local interfacial electrochemical activity^[40]. A schematic summary of the proposed structural evolution is provided in Supplementary Figure 13 [Supplementary Materials]. The Cu(II)-to-Cu(I) reduction associated with this reconstruction is a Faradaic process with a finite charge contribution. Complete one-electron reduction corresponds to a theoretical capacity of approximately 176.8 mAh g^-1 of CuC₂O₄, equivalent to an upper-bound contribution of ~3.54 mAh g^-1 for the electrode containing 2 wt% CuC₂O₄. This finite reconstruction-related charge is therefore distinct from continuously accumulating parasitic charge consumption associated with hydrogen evolution and corrosion. Within the scope of the present evidence, the resulting C-O-enriched and Cu(I)-related interfacial environment is considered to be largely retained during subsequent cycling rather than undergoing a complete Cu(II)/Cu(I) and C=O/C-O reversal in each plating/stripping cycle.

After this phase transition, the newly generated C-O-enriched and Cu⁺-related surface no longer merely represents a changed copper oxalate structure, but instead functions as a reconstructed interfacial coordination environment for subsequent H₂O and Zn²⁺ regulation. To clarify this second mechanistic component, density functional theory (DFT) calculations were performed to evaluate the adsorption behavior of H₂O and Zn²⁺ at different coordination sites. Here, Zn²⁺ represents the desolvated ionic species after removal of its explicit hydration shell, rather than a hydrated [Zn(H₂O)_x]²⁺ complex. For H₂O adsorption, the calculated adsorption energies at the five representative sites were generally more negative on the C-O sites than on the C=O sites, indicating stronger interactions with H₂O molecules on the post-transition C-O-enriched interface [Figure 4G]. Calculations for the copper sites further indicate that Cu⁺ exhibits stronger interactions with H₂O than Cu²⁺ [Figure 4H], suggesting that the reconstructed interface is more capable of constraining interfacial water molecules. A similar trend was observed for Zn²⁺ adsorption. The average adsorption energy of Zn²⁺ at single-bond oxygen sites (C-O) is -0.1299 eV, which is lower than the -0.0772 eV obtained at carbonyl oxygen sites (C=O), indicating stronger Zn²⁺ binding on the C-O-rich interface [Figure 4I]. Meanwhile, the fluctuation range and standard deviation of the adsorption energies on the C-O sites are both smaller than those on the C=O sites, indicating that Zn²⁺ adsorption in the C-O environment is not only stronger, but also more spatially uniform. In addition, adsorption calculations for different metal centers show that the Cu⁺ site exhibits the strongest binding to Zn²⁺, significantly outperforming the Cu²⁺ site and the Zn substrate [Figure 4J]. It should be emphasized that these adsorption energies describe the affinity of ionic Zn²⁺ toward the reconstructed interface prior to electrochemical reduction and therefore should not be interpreted as the binding energy of metallic Zn or as the kinetic barrier for subsequent Zn stripping. Thus, the enhanced Zn²⁺ affinity primarily facilitates more favorable and homogeneous Zn²⁺ adsorption and nucleation during plating, but does not necessarily imply inhibited removal of metallic Zn during stripping. These results indicate that the phase transition of CuC₂O₄ further induces an interfacial coordination reconstruction that modulates the interaction with H₂O and Zn²⁺. The reconstructed interface exhibits stronger water-confinement capability and higher zinc-affinity compared to the pristine surface. This coordination environment promotes more uniform Zn²⁺ adsorption and desolvation, contributing to the enhanced electrochemical stability of the zinc powder anode. It should be noted that the H₂O and Zn²⁺ adsorption energies were calculated independently and therefore should not be directly compared to infer competitive occupation of the same Cu⁺ site. The simultaneous enhancement of water confinement and zinc affinity does not indicate indiscriminate adsorption. Instead, the C-O-enriched environment can immobilize interfacial water through hydrogen-bonding/coordination interactions, thereby reducing the activity of free water toward parasitic reduction, while the Cu⁺-related sites and oxygen-rich coordination environment provide more uniform Zn²⁺ adsorption sites. This dual regulation suppresses competitive water reduction while guiding homogeneous Zn deposition.

To further evaluate the practical applicability of ZP@CuC₂O₄, we assembled Zn//V₂O₅ full cells to assess its potential for real-world applications. The cyclic voltammetry curves show that the voltage gap decreases from 0.236 V for the ZP cell to 0.198 V for the ZP@CuC₂O₄ cell [Figure 5A], indicating accelerated Zn²⁺/V⁵⁺ redox kinetics and reduced polarization. The modified full cell also delivers superior rate capability over 1-10 A g^-1 [Figure 5B]. During long-term cycling, it retains 82 mAh g^-1 after 2,000 cycles at 5 A g^-1 [Figure 5C], while the pristine ZP cell undergoes rapid capacity decay within 520 cycles. At 7 A g^-1, the ZP@CuC₂O₄-based full cell also maintains stable capacity output with a coulombic efficiency close to 90%, whereas the bare ZP system fails much earlier [Supplementary Figure 14, Supplementary Materials]. Even at 10 A g^-1, a reversible capacity of 78 mAh g^-1 is retained after 3,600 cycles, far beyond the 1,100-cycle lifetime of the control [Figure 5D]. The advantage remains evident at 15 A g^-1 as well [Supplementary Figure 15, Supplementary Materials]. Post-cycling SEM and elemental mapping further show that the modified anode preserves a dense and uniform surface after prolonged operation [Figure 5E, Supplementary Figure 16 and Supplementary Table 2, Supplementary Materials], consistent with the enhanced interfacial stability inferred from preceding results.

The robustness of the reconstructed interface is also maintained under elevated temperature and practical device configurations. Elevated temperature generally intensifies water-related parasitic reactions and interfacial instability of zinc anodes^[41,42]. At 40 °C, the ZP@CuC₂O₄ full cell still exhibits stable cycling at different current densities, whereas the control cell cannot sustain normal operation [Figure 5F, Supplementary Figures 17-19, Supplementary Materials]. This indicates that the restructured interface induced by CuC₂O₄ not only buffers local polarization and side reactions at room temperature but also effectively suppresses interfacial instability caused by accelerated reactions under high-temperature conditions. To further verify scalability, a 5 cm × 5 cm pouch cell was assembled using the ZP@CuC₂O₄ electrode. The device shows an open-circuit voltage of 1.274 V [Figure 5G] and can directly power a digital watch [Figure 5H], demonstrating clear output capability. Under a cathode loading of 5.72 mg cm^-2, the pouch cell operates stably for 350 cycles at 3 A g^-1, with a cumulative discharge capacity of 5.5 Ah [Figure 5I]. Under a cathode loading of 4.68 mg cm^-2, it sustains excellent cycling for 1,000 cycles at 7 A g^-1, reaches a peak discharge capacity of 225 mAh g^-1, and delivers a cumulative capacity of 11.7 Ah [Figure 5J]. The key practical parameters of the pouch cells, including negative-to-positive electrode capacity (N/P) ratio, Zn-anode depth of discharge (DOD), electrolyte volume-to-capacity (E/C) ratio, initial discharge capacity, and capacity retention, are summarized in Supplementary Table 3 [Supplementary Materials]. The transient apparent CE above 100% during the initial cycles of the pouch cell is likely associated with a non-steady-state activation process, during which progressive electrolyte wetting and cathode/interfacial activation cause the accessible discharge capacity to increase more rapidly than the corresponding charge capacity. As the ion-transport pathways and electrode contacts gradually stabilized, the coulombic efficiency rapidly recovered and remained close to 100%, indicating that the cell subsequently entered a stable cycling regime. These results collectively confirm the strong high-rate adaptability, thermal tolerance, and practical application potential of the ZP@CuC₂O₄ anode. To further evaluate the compatibility of the modified Zn anode beyond the V₂O₅ cathode chemistry, ZP@CuC₂O₄ was coupled with an I₂ cathode, and the resulting Zn//I₂ full cells exhibited reversible cycling at 2 and 5 A g^-1 [Supplementary Figure 20, Supplementary Materials].

This study demonstrates a phase transformation-driven interfacial coordination reconstruction strategy to mitigate the thermodynamic instability of zinc powder anodes in aqueous zinc-ion batteries. The transformation, characterized by the evolution of the carbon-oxygen framework and copper valence states, facilitates the formation of a robust interphase rich in C-O coordination and Cu⁺-related active sites. This dynamically evolved interface effectively regulates Zn²⁺ flux and deposition kinetics, thereby mitigating side reactions and “dead zinc” formation. The ZP@CuC₂O₄ anode demonstrates superior cycling stability under high-rate conditions and maintains high capacity in full cells across a range of temperatures. The strategy of achieving “active regulation” through internal chemical reconstruction provides an alternative approach for stabilizing zinc powder anodes, addressing a key barrier toward practical aqueous zinc-ion batteries.