Zinc Metal Anode Research Articles

Electrode/Electrolyte Optimization-Induced Double-Layered Architecture for High-Performance Aqueous Zinc-(Dual) Halogen Batteries

HighlightsA double-layered protective film based on zinc-based coordination compound and ZnF2-rich solid electrolyte interphase layer has been successfully fabricated on the zinc metal anode via electrode/electrolyte synergistic optimization.The double-layered architecture can effectively modulate Zn2+ flux and suppress the zinc dendrite growth, thus facilitating the uniform zinc deposition.The as-developed zinc-(dual) halogen batteries based on double-layered protective film can present high areal capacity and satisfactory cycling stability.

Synergistic Regulation of Anode and Cathode Interphases via an Alum Electrolyte Additive for High‐Performance Aqueous Zinc‐Vanadium Batteries

AbstractA zinc (Zn) metal anode paired with a vanadium oxide (VOx) cathode is a promising system for aqueous Zn–ion batteries (AZIBs); however, side reactions proliferating on the Zn anode surface and the infinite dissolution of the VOx cathode destabilise the battery system. Here, we introduce a multi‐functional additive into the ZnSO4 (ZS) electrolyte, KAl(SO4)2 (KASO), to synchronise the in situ construction of the protective layer on the surface of the Zn anode and the VOx cathode. Theoretical calculations and synchrotron radiation have verified that the high‐valence Al3+ plays dual roles of competing with Zn2+ for solvation and forming a Zn−Al alloy layer with a homogeneous electric field on the anode surface to mitigate the side reactions and dendrite generation. The Al‐containing cathode–electrolyte interface (CEI) considerably alleviates the irreversible dissolution of the VOx cathode and the accumulation of byproducts. Consequently, the Zn||Zn cell with KASO exhibits an ultra‐long cycle of 6000 h at 2 mA cm−2. Importantly, the VOx cathodes (VO2, V2O5 and NH4V4O10) in the ZS−KASO electrolyte showed excellent cycling stability, including Zn powder||VO2 cells and Zn||VO2 pouch cells. Even better, the full cell exhibits excellent cycling stability at low negative/positive (N/P) ratio of 2.83 and high mass loading (~16 mg cm−2). This study offers a straightforward and practical reference for concurrently addressing challenges at the anode and cathode of AZIBs.

A Synergistic Zincophilic and Hydrophobic Supramolecule Shielding Layer for Actualizing Long‐Term Zinc‐Ion Batteries

AbstractThe zinc metal anodes are liable to experience detrimental dendrite growth and side reactions, thereby limiting the lifespan of aqueous Zn‐ion batteries. Here, a readily available supramolecule, dimethoxypillar[5]arene (DP[5]), is utilized as a shielding layer to stabilize the Zn anode by exploiting its zincophilicity derived from the ─OCH3 functional groups and its hydrophobicity from the hydrophobic backbone. The DP[5] shielding layer regulates the solvation sheath of Zn2+ and facilitates uniform zinc deposition. Swelling and dendrite formation are obviously suppressed in both the symmetric and full cells. The DP[5]‐Zn symmetrical cell cycles stably for 5500 h, and achieves a coulombic efficiency of 99.76% in a DP[5]‐Zn||Cu half‐cell after 2200 cycles. The DP[5]‐Zn||V2O5 full cell maintains 92.03% of initial capacity after 6000 cycles. Given the cost‐effective fabrication and environmental friendliness of DP[5] films, this material may pave the way for practical applications of zinc anodes.

Breath inspired multifunctional low-cost inorganic colloidal electrolyte for stable zinc metal anode

The practical application of aqueous zinc-ion batteries (AZIBs) is primarily constrained by issues such as corrosion, zinc dendrite formation, and the hydrogen evolution reaction occurring at the zinc metal anode. To overcome these challenges, strategies for optimizing the electrolyte are crucial for enhancing the stability of the zinc anode. Inspired by the role of hemoglobin in blood cells, which facilitates oxygen transport during human respiration, an innovative inorganic colloidal electrolyte has been developed: calcium silicate-ZnSO4 (denoted as CS-ZSO). This electrolyte operates in weak acidic environment and releases calcium ions, which participate in homotopic substitution with zinc ions, while the solvation environment of hydrated zinc ions in the electrolyte is regulated. The reduced energy barrier for the transfer of zinc ions and the energy barrier for the desolvation of hydrated ions imply faster ion transfer kinetics and accelerated desolvation processes, thus favoring the mass transfer process. Furthermore, the silicate colloidal particles act as lubricants, improving the transfer of zinc ions. Together, these factors contribute to the more uniform concentration of zinc ions at the electrode/electrolyte interface, effectively inhibiting zinc dendrite formation and reducing by-product accumulation. The Zn//CS-ZSO//Zn symmetric cell demonstrates stable operation for over 5000 h at 1 mA cm−2, representing 29-fold improvement compared to the Zn//ZSO//Zn symmetric cell, which lasts only 170 h. Additionally, the Zn//CS-ZSO//Cu asymmetric cell shows stable average Coulombic efficiency (CE) exceeding 99.6% over 2400 cycles, significantly surpassing the performance of the ZSO electrolyte. This modification strategy for electrolytes not only addresses key limitations associated with zinc anodes but also provides valuable insights into stabilizing anodes for the advancement of high-performance aqueous zinc-ion energy storage systems.

High-viscoelasticity alginate-based coatings for reversible zinc metal anodes

High-safety aqueous zinc (Zn) ion batteries are troubled by dendrite growth and hydrogen evolution reaction on Zn anode, which can be well solved via the construction of surface protective layer. The recent researches mainly focus on the bulk property of the protective layer, but its separation from Zn anode is ignored. In this work, high-viscoelasticity alginate-based (HVAA) layer was in-situ constructed on Zn anodes by the cross-linking of sodium alginate with formaldehyde and the plastifying of glycerin. HVAA layer can combine with H2O and coordinate with Zn2+ ions in aqueous electrolyte to achieve viscoelasticity on Zn anode, which can accommodate volume change of Zn anode during plating/stripping processes to continuously protect Zn anodes under the real battery system. Physical block effect of HVAA layer impedes hydrogen evolution corrosion reaction by avoiding the immediate contact of Zn anodes with aqueous electrolyte. Ionic conductive ability of HVAA layer by coordinating oxygen-containing groups with Zn2+ can uniform ion flux to induce the homogeneous deposition of Zn2+ on Zn anode. Zn anode with HVAA endows ZnZn symmetric battery with stably cycle of 4000 h and Zn-iodide full batteries with better electrochemical performance of 8000 cycles comparing with bare Zn anode. This work opens a novel route to continuously protect Zn anode through the high-viscoelasticity films to closely fit with Zn surface and implement the high-value application of renewable sources.

Bifunctional Ion Rectification Layer Separators Toward Superior Reversible Dendrite‐Free Zinc Metal Anodes

AbstractThe slow transport dynamics and poor dendritic growth significantly hinder the performance of zinc metal batteries. Here, a unique difunctional ion rectification strategy is developed using vacuum evaporation technology to design a coated separator for efficient ion transport. The highly conductive Cu‐coated separator acts as an ion redistributor, ensuring homogenized electric field distribution. The excellent znophilicity of the copper coating acts as an ion accelerator, promoting ion transport and facilitating face‐to‐face zinc deposition on the separator. Consequently, this synergy enables stable battery operation at high current densities (cumulative capacity up to 10 800 mAh cm−2 at 8 mA cm−2) and high depth of discharge (over 200 h at 94% DOD). The Cu‐coated separator exhibits a reversible plating/stripping life of over 2400 h with an average coulombic efficiency of 99.88%. Notably, the Cu‐coated separator significantly enhances the rate performance and cycle capacity of Zn||V6O13 and Zn||MnO2 full cells. This functional separator with a difunctional ion rectification strategy presents a promising solution to the challenge of zinc metal anodes.

Innovative Zinc Anodes: Advancing Metallurgy Methods to Battery Applications.

Aqueous zinc metal batteries (AZMBs) are emerging as a powerful contender in the realm of large-scale intermittent energy storage systems, presenting a compelling alternative to existing ion battery technologies. They harness the benefits of metal zinc's high safety, natural abundance, and favorable electrochemical potential (-0.762V vs Standard hydrogen electrode, SHE), alongside an impressive theoretical capacity (820mAhg-1 and 5655mAhcm-3). However, the electrochemical performance of ZMBs is impeded by several challenges, including poor compatibility with high-loading cathodes and persistent side reactions. These issues are intricately linked to the inherent physicochemical properties of the zinc metal anodes (ZMAs). Here, this review delves into the traditional methods of ZMAs production, encompassing extraction, electrodeposition, and rolling processes. The discussion then progresses to an exploration of cutting-edge methodologies designed to enhance the electrochemical performance of ZMAs. These methods are categorized into alloying, pre-treatment of substrate, advanced electrodeposition techniques, and the development of composite anodes utilizing zinc powder. The review offers a comparative analysis of the merits and drawbacks of various optimization strategies, highlighting the beneficial outcomes achieved. It aspires to inspire novel concepts for the advancement and innovation of next-generation zinc-based energy storage solutions.

Modification of Cu-Based Current Collectors and Their Application in High-Performance Zn Metal Anode: A Review

Zinc-based batteries (ZBBs) have proven to be tremendously plausible for large-scale electrochemical energy storage applications due to their merits of desirable safety, low-cost, and low environmental impact. Nevertheless, the zinc metal anodes in ZBBs still suffer from many issues, including dendrite growth, hydrogen evolution reactions (HERs), corrosion, passivation, and other types of undesirable side reactions, which severely hinder practical application. The modification of Cu-based current collectors (CCs) has proven to be an efficient method to regulate zinc deposition and prevent dendritic growth, thereby improving the Coulombic efficiency (CE) and lifespan of batteries (e.g., up to 99.977% of CE over 6900 cycles after modification), which is an emerging research topic in recent years. In this review, we provide a systematic overview of the modification of copper-based CCs and their application in zinc metal anodes. The relationships between their modification strategies, nano-micro-structures, and electrochemical performance are systematically reviewed. Ultimately, their promising prospects for future development are also proposed. We hope that this review could contribute to the design of copper-based CCs for zinc-based batteries and facilitate their practical application.

Dynamically Favorable Ion Channels Enabled by a Hybrid Ionic-Electronic Conducting Film toward Highly Reversible Zinc Metal Anodes.

Aqueous zinc ion batteries show great promise for future applications due to their high safety and ecofriendliness. However, nonuniform dendrite growth and parasitic reactions on the Zn anode have severely impeded their use. Herein, a hybrid ionic-electronic conducting ink composed of graphene-like carbon nitride (g-C3N4) and conductive polymers (CP) of poly(3,4ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS) is introduced to Zn anode using a scalable spray-coating strategy. Notably, the g-C3N4 promotes a screening effect, disrupting the coulombic interaction between the PEDOT+ segments and PSS- chains within CP, thereby reducing interfacial resistance and homogenizing the surface electric field distribution of the Zn anode. Furthermore, the abundant N-containing species and ─SO3 - groups in g-C3N4/CP exhibit strong zincophilicity, which accelerates the diffusion of Zn2+ and disrupts the solvation structure of Zn(H2O)6 2+, thus improving the Zn2+ transfer capability. Consequently, the g-C3N4/CP can powerfully stabilize the Zn2+ flux and thus enable a high coulombic efficiency of 99.47% for 1500 cycles and smooth Zn plating/stripping behaviors more than 3000h at a typical current density of 1mA cm-2. These findings shed new light on the Zn electrodeposition process under the mediation of g-C3N4/CP and offer sustainability considerations in designing more stable Zn-metal anodes with enhanced reversibility.

Mechanical Grinding Formation of Highly Reversible (002)‐Textured Zinc Metal Anodes

AbstractThe practical applications of zinc metal anode are restricted by detrimental dendrite growth and hydrogen evolution reaction (HER), especially at high current densities. Previous works have demonstrated that constructing Zn(002) texture could effectively suppress dendrite growth and HER. However, the surface grain distribution of commercial zinc metal remains indistinct. Herein, a simple mechanical grinding approach is demonstrated to construct (002)‐textured zinc metal anodes. After grinding, the (002) relative texture coefficient of commercial zinc metal increases from 10.58 to 42.28, indicating a significant more (002) planes exposure. As prepared (002)‐textured zinc anode exhibits a high critical current density of 141 mA cm−2 and stably cycles for over 1500 cycles at 50 mA cm−2 and 1 mAh cm−2. Benefiting from the stability and fast kinetics of this (002)‐textured zinc anode, the zinc‐ion capacitor achieves a power density of 8500 W kg−1 and long cycle over 10 000 cycles with Coulombic efficiency (CE) exceeding 99.9%. This work provides both fundamental and practical insights for dendrite‐free and HER‐suppressed zinc metal anodes and inspiring guidance for other metal batteries.

Stable and reversible zinc metal anode with fluorinated graphite nanosheets surface coating

A highly stable zinc metal anode modified with a fluorinated graphite nanosheets (FGNSs) coating was designed. The porous structure of the coating layer effectively hinders lateral mass transfer of Zn ions and suppresses dendrite growth. Moreover, the high electronegativity exhibited by fluorine atoms creates an almost superhydrophobic solid−liquid interface, thereby reducing the interaction between solvent water and the zinc substrate. Consequently, this leads to a significant inhibition of hydrogen evolution corrosion and other side reactions. The modified anode demonstrates exceptional cycling stability, as symmetric cells exhibit sustained cycling for over 1400 h at a current density of 5 mA/cm2. Moreover, the full cells with NH4V4O10 cathode exhibit an impressive capacity retention rate of 92.2% after undergoing 1000 cycles.

Zwitterion Modified Polyacrylonitrile Fiber Separator for Long‐Life Zinc‐Ion Batteries

AbstractThe major challenges of aqueous zinc‐ion batteries (ZIBs) are the dendrite formation and the passivation of zinc metal anode, which restrict their practical applications. Herein, polyacrylonitrile (PAN) and zwitterionic surfactant (Sulfobetaine methacrylate, SBMA) are combined as a precursor to design a modified PAN nanofiber separator by electrospinning. SBMA with sulfonate group [SO3−] can alter the physical property of the precursor solution and electrostatic field during the electrospinning process. Besides, it can regulate the zinc ions crossing and homogenize the electric field by minimizing the zinc ion concentration polarization on the zinc foil surface due to the polar group. As a result, Zn symmetric cells with PAN@SBMA separators show long‐term stability (up to 1700 h), which outdistances the cell with GF‐D (only up to 50 h) under current density at 1 mA cm−2. Meanwhile, the Zn//PAN@SBMA//NH4V4O10 full cells have high specific capacity (236 mAh g−1) and excellent long‐term durability with 84.2% capacity retention after 2000 cycles at 5 A g−1. This work illustrates an easy and effective way to design a high ion transference number and functional PAN‐based separator for regulating Zn2+ deposition for the development of high‐performance ZIBs.

Electrical Double Layer and In Situ Polymerization SEI Enables High Reversible Zinc Metal Anode.

Aqueous zinc-ion batteries (AZIBs) stand out among new energy storage devices due to their excellent safety and environmental friendliness. However, the formation of dendrites and side reactions on the zinc metal anode during cycling have become the major obstacles to their commercialization. This study innovatively selected Sodium 4-vinylbenzenesulfonate (VBS) as a multifunctional electrolyte additive to address the issues. The dissociated VBS- anions can not only significantly alter the hydrogen bond network structure of H2O in the electrolyte, but also preferentially adsorb on the surface of the zinc anode before H2O molecules, which will result in the development of organic anion-rich interface and alterations to the electrical double layer (EDL) structure. Furthermore, the ─C═C─ structure in VBS leads to the formation of an in situ polymerized organic anion solid electrolyte interface (SEI) layer that adheres to the surface of the zinc anode. The mechanisms work together to significantly improve the performance of Zn//Zn symmetric batteries, achieving a cycle life of over 1800h at 1mA cm-2 and 1 mAh cm-2. The introduction of VBS also enhances the cycling performance and capacity of Zn//δ-MnO2 full cells. This study provides a low-cost solution for the development of AZIBs.

Synergistic Gradient Anodes for Long-Term Stability in Aqueous Zinc-Ion Batteries.

The stability of aqueous zinc metal anodes is still constrained by their severe dendrite growth. Optimizing electric field distribution and crystallography to modulate the diffusion and deposition behavior of zinc ions can effectively suppress dendrite growth. However, the fabrication strategy to directly endow specific textured zinc anodes with gradient electric field distribution is still lacking. Herein, a strategy combining crystal reconstruction of commercial zinc foil with graphene oxide (GO) protective layer is proposed to construct an in situ gradient electric field-enhanced strong (002) textured GO@ZnO/Zn(002) anode. Based on the experimental and theoretical results, the GO protective layer can regulate a wide-range homogeneous Zn2+ ions flow, while the dense and uniform ZnO/Zn(002) nanoneedles /nanoparticles can enhance localized polarized electric field to accelerate rapid localized transfer of Zn2+ ions and guide them toward directional deposition along (002) plane. Therefore, the hierarchical GO@ZnO/Zn(002) anode enables the symmetric cell to operate continuously and stably for 5700 and 4200h at 2 and 4mA cm-2, respectively, which is comparable to or better than most high-end Zn anodes. This work presents new insights into the zinc foil reconstruction and gradient electric field fabrication strategy, offering a scalable approach for the development of long-term stable metal anodes.

Synergistic Regulation of Anode and Cathode Interphases via an Alum Electrolyte Additive for High-Performance Aqueous Zinc-Vanadium Batteries.

A zinc (Zn) metal anode paired with a vanadium oxide (VOx) cathode is a promising system for aqueous Zn-ion batteries (AZIBs); however, side reactions proliferating on the Zn anode surface and the infinite dissolution of the VOx cathode destabilise the battery system. Here, we introduce a multi-functional additive into the ZnSO4 (ZS) electrolyte, KAl(SO4)2 (KASO), to synchronise the in situ construction of the protective layer on the surface of the Zn anode and the VOx cathode. Theoretical calculations and synchrotron radiation have verified that the high-valence Al3+ plays dual roles of competing with Zn2+ for solvation and forming a Zn-Al alloy layer with a homogeneous electric field on the anode surface to mitigate the side reactions and dendrite generation. The Al-containing cathode-electrolyte interface (CEI) considerably alleviates the irreversible dissolution of the VOx cathode and the accumulation of byproducts. Consequently, the Zn||Zn cell with KASO exhibits an ultra-long cycle of 6000 h at 2 mA cm-2. Importantly, the VOx cathodes (VO2, V2O5 and NH4V4O10) in the ZS-KASO electrolyte showed excellent cycling stability, including Zn powder||VO2 cells and Zn||VO2 pouch cells. Even better, the full cell exhibits excellent cycling stability at low negative/positive (N/P) ratio of 2.83 and high mass loading (~16 mg cm-2). This study offers a straightforward and practical reference for concurrently addressing challenges at the anode and cathode of AZIBs.

Electric Field Regulator Constructed by Magnetron Sputtering for Dendrite‐Free and Stable Zinc Metal Anode

AbstractRechargeable aqueous zinc‐ion batteries (AZIBs) are considered to be one of the most promising devices in the next generation of energy storage systems. However, the uncontrolled growth of Zn dendrites during electroplating leads to rapid battery failure, which hinders the wide application of AZIBs. In this work, an Fe metal interface (FMI) with electric field regulation is designed on the Zn metal anode using a magnetron sputtering technology. The FMI layer with nanosheet array not only uniforms the surface electric field, but also adjusts the surface Zn2+ ion distribution to inhibit 2D diffusion. The strong orientation relationships of the FMI layer enhance the reversibility of Zn plating/stripping, improving the structural stability of the interface layer. Consequently, FMI@Zn symmetric cell exhibits ultra‐stable lifespan for over 6000 h (Cumulative plated capacity, CPC = 15 Ah cm−2) with a low voltage hysteresis of 46.4 mV and high Coulombic efficiency of 99.8% at 5 mA cm−2. Even at the large current density of 40 mA cm−2, the CPC reaches 19.7 Ah cm−2. The proposed electric field regulation strategy reveals a promising prospect for designing highly stable Zn anode, which also applies to other metal anodes in energy storage systems.

Steric hindrance and orientation polarization by a zwitterionic additive to stabilize zinc metal anodes

AbstractZinc metal stands out as a promising anode material due to its exceptional theoretical capacity, impressive energy density, and low redox potential. However, challenges such as zinc dendrite growth, anode corrosion, and side reactions in aqueous electrolytes significantly impede the practical application of zinc metal anodes. Herein, 3‐(1‐pyridinio)‐1‐propanesulfonate (PPS) is introduced as a zwitterionic additive to achieve long‐term and highly reversible Zn plating/stripping. Due to the orientation polarization with the force of electric field, PPS additive with π–π conjugated pyridinio cations and strong coordination ability of sulfonate anion tends to generate a dynamic adsorption layer and build a unique water–poor interface. PPS with steric hindrance effect and strong coordination ability can attract solvated Zn2+, thereby promoting the desolvation process. Moreover, by providing a large number of nucleation sites and inducing zinc ion flow, the preferred orientation of the (002) crystal plane can be achieved. Therefore, the interfacial electrochemical reduction kinetics is regulated and uniform zinc deposition is ensured. Owing to these advantages, the Zn//Zn symmetrical cell with PPS additive exhibits remarkable cycling stability exceeding 2340 h (1 mA cm−2 and 1 mA h cm−2). The Zn//V2O5 full cell also delivers stable cycling for up to 6000 cycles.

Cobalt-doped copper sulfide nanocomposite integrated with graphene oxide as a high-performance conversion anode for aqueous zinc-ion batteries

Rechargeable aqueous zinc-ion batteries (ZIBs) encounter substantial obstacles arising from the inherent dilemmas of dendrite growth, hydrogen gas evolution, and corrosion affiliated with zinc metal anodes, thereby highlighting the necessity for researching conversion anode materials as a promising pathway forward. Copper sulfide (CuS) has been demonstrated as a promising conversion anode material for ZIBs due to its notable electrochemical performance, while challenges persist regarding the Coulombic interactions between Zn2+ and host anions, coupled with the material’s fundamental conductivity that remains less than fully satisfactory. To address the above issues, we have designed and synthesized a nanostructured composite of cobalt doped CuS integrated in graphene oxide frames (GO/Co-CuS) as anode for ZIBs. The cobalt doping serves to alleviate Coulomb interaction (Coulomb attraction) between Zn2+ and host anions, thereby enhancing the kinetics of Zn2+ diffusion. Furthermore, the incorporation of GO framework improves the electrical conductivity of the material and mitigates volume expansion during the reaction process. The synergistic effect engendered by the combination of cobalt doping and the incorporation of a GO framework results in the remarkable electrochemical performance exhibited by GO/Co-CuS. The GO/Co-CuS composite nanostructure exhibited commendable rate capability and cycling stability. Specifically, it exhibits remarkable rate capability, delivering 296 mAh g−1 at 1 A/g and 168 mAh g−1 at 10 A/g. Furthermore, after 1000 cycles at a high current density of 10 A/g, it maintains a capacity of 166 mAh g−1, demonstrating exceptional cycling stability. Additionally, the full-cell configuration of GO/Co-CuS//MnO2@CNTs, when cycled 241 times at 2 A/g, retains a capacity of 79 mAh g−1, thereby confirming the practical efficacy of the GO/Co-CuS nanocomposite as an efficient conversion anode for ZIBs.

Targeting inerratic deposition behaviour via interface regulation toward dendrite-free zinc metal anodes

Aqueous zinc ion batteries are of interest due to their inherent safety, low cost and high energy density. Nevertheless, critical issues such as uncontrollable dendrite growth, hydrogen evolution reaction and corrosion have dramatically impeded the widespread utilization. To tackle above issues, the versatile artificial protective layer strategy consisting of Zn-friendly, porous and conductive carbon shells is presented for yolk-shell SiO2@void@C (SVC) nanospheres for guiding rapid and homogeneous Zn plating/stripping. On the one hand, the highly zincophilic SiO2 and pore structure interacted significantly with low nucleation overpotential and uniform Zn2+ flux, which favored homogeneous zinc deposition and ionic migration, thereby dramatically aiding in inhibition of Zn dendrites and interruption of interfacial side reactions. On the other hand, SVC nanospheres confer excellent electrical conductivity and mechanical properties, which play an important role in accelerating ion diffusion and boosting structural stability. Consequently, the SVC@Zn electrode exhibits high reversibility and electrochemical stability with a long cycling stability of 1800 h at 5 mA cm−2/1.25 mAh cm−2 and average CE of 99 %. The good properties associated with composition simplicity and abundant yield affords a feasible scheme for high-performance AZIBs.

Motional Resistance as Highly Selective Descriptor to Probe Dynamic Formation of Surface Films on Zinc Anode

AbstractZinc anodes are expected as a promising alternative to lithium‐based anodes in energy storage systems due to their low cost, high theoretical capacity, and environmental friendliness. However, the development of efficient and stable zinc anode requires a fundamental understanding of the interfacial processes occurring during zinc deposition and dissolution cycling. In this study, we employed electrochemical quartz crystal microbalance (EQCM) analysis to investigate the potential‐dependent formation and decomposition of surface films on zinc metal anodes in sulfate‐based aqueous electrolytes. Changes in frequency and motional resistance served as complementary descriptors, with motional resistance being a highly selective indicator for probing dynamic surface film formation driven by side reactions at the zinc anode. While the frequency change provided the overall changes in the mass of both zinc metal and surface films, changes in the motional resistance selectively reflected the amount and nature of the visco‐elastic interface that comprise the surface films. The two descriptors provide quantitative and complementary means to discover the complex interfacial processes such as the formation of surface visco‐elastic films, guiding to the development of more stable and efficient zinc‐based electrochemical systems.