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Zinc ion batteries (ZIBs) suffer from severe corrosion effects and dendrite growth on the unstable anode/electrolyte interface (AEI) during the plating/stripping process. Therefore, it is of great significance to build a stable AEI enabling a long lifetime for ZIBs. Herein, trace tea polyphenols (TP) were introduced firstly as additive of zinc acetate electrolyte to protect zinc anode from corrosion invasion and boost uniform zinc deposition, thus achieving reversible dendrite-free zinc anode. In situ synchrotron radiation X-ray imaging was conducted to illustrate the positive role of TP molecules in the uniform plating process of zinc. The stable AEI induced by the specific adsorption of TP molecules reduced hydrogen and oxygen evolution side reactions and increased the coulombic efficiency. The TP additive with an ultralow dosage of 0.028 g L -1 delivered favorable cycling stability of 720 h at 0.5 mA cm -2 and 0.5 mAh cm -2 . The Zn-Na 3 V 2 (PO 4 ) 3 full cell assembled with the hybrid Zn(Ac) 2 -TP electrolyte contributed an energy density of 130 mAh g -1 at the current density of 0.2C and enhanced cycling stability of 78% retention after 300 cycles. These results will provide new insights into additive engineering for aqueous electrolytes and the fundamental understanding of AEI phenomena for high performance ZIBs., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier Inc. All rights reserved.)

A separator modification strategy was proposed by placing nitrogen-doped carbon fibers (NCF700) in the middle of the separator to prevent direct contact between the coating and the rigid zinc metal anode, resulting in coating cracks. The NCF700 coating can homogenize the electric field distribution and increase the transference number of zinc ions. Therefore, the battery assembled with the NCF700 coated separator exhibits superior cycling stability compared to the bare separator. [ABSTRACT FROM AUTHOR]

The Zn metal anode is subject to uncontrolled dendrites and parasitic reactions, which often require a big thickness of Zn foil, resulting in excess capacity and extremely low utilization. Here, an ultrathin Zn composite anode (24 µm) is developed with a protective hydrophobic layer (covalent (C2F4)n chains and F‐doped carbonized ingredient) constructed on Cu foil (denoted as (C2F4)n‐C@Cu) as a host by one‐step pyrolytic evaporation deposition. The repulsion of (C2F4)n to Zn2+ makes the (C2F4)n‐C@Cu interface possess enhanced adsorption ability, driving more charge transfer under the layer. With its good hydrophobicity, this layer prevents H2O from damaging the plated Zn. Combined with the semi‐ionic‐state fluorine as zincophilic site, the host guides uniform and dense Zn deposition for making ultrathin Zn anode. As a result, the (C2F4)n‐C@Cu electrode exhibits high average CE of 99.6% over 3000 cycles at 2 mA cm−2. Benchmarked against the commercial 20µm‐Zn foil, the (C2F4)n‐C@Cu@Zn anode achieves enhanced stability (1200 h at 1 mA cm−2), only 100 h for the 20µm‐Zn foil. When paired with V2O5 cathode, the Zn composite anode makes the full cell deliver 88% retention for 2500 cycles. [ABSTRACT FROM AUTHOR]

High‐voltage aqueous rechargeable energy storage devices with safety and high specific energy are hopeful candidates for the future energy storage system. However, the electrochemical stability window of aqueous electrolytes is a great challenge. Herein, inspired by density functional theory (DFT), polyethylene glycol (PEG) can interact strongly with water molecules, effectively reconstructing the hydrogen bond network. In addition, N, N‐dimethylformamide (DMF) can coordinate with Zn2+, assisting in the rapid desolvation of Zn2+ and stable plating/stripping process. Remarkably, by introducing PEG400 and DMF as co‐solvents into the electrolyte, a wide electrochemical window of 4.27 V can be achieved. The shift in spectra indicate the transformation in the number and strength of hydrogen bonds, verifying the reconstruction of hydrogen bond network, which can largely inhibit the activity of water molecule, according well with the molecular dynamics simulations (MD) and online electrochemical mass spectroscopy (OEMS). Based on this electrolyte, symmetric Zn cells survived up to 5000 h at 1 mA cm−2, and high voltage aqueous zinc ion supercapacitors assembled with Zn anode and activated carbon cathode achieved 800 cycles at 0.1 A g−1. This work provides a feasible approach for constructing high‐voltage alkali metal ion supercapacitors through reconstruction strategy of hydrogen bond network. [ABSTRACT FROM AUTHOR]

Aqueous zinc batteries usher in a renaissance due to their intrinsic security and cost effectiveness, bespeaking vast application foreground for large‐scale energy storage system. However, uncontrolled dendrite growth along with hydrogen evolution severely restricts its reversibility and stability for practical application. Herein, the surface of Zn metal is reconstructed with metallic particles (In, Sn, In0.2Sn0.8) to diminish surface defects and regulate Zn deposition behavior. The alloyed In–Sn greatly activates the Zn surface for lower Zn adsorption energy barrier to expedite plating kinetics and confine Zn aggregation. Dense and uniform deposition of Zn on the reconstructed surface significantly prevents the Zn substrate from dendrites growth for catastrophic damage. Meanwhile, alloy layer embodies high hydrogen evolution overpotential, ensuring high plating and stripping efficiency for Zn anode. Consequently, In0.2Sn0.8 reconstructed surface realizes long‐term lifespan up to 1800 h with low polarization (12 mV) at the condition of 1 mA cm−2 and 1 mAh cm−2. When paired with sodium vanadate (NVO) cathode, the full cell steady operates for a high‐capacity retention of 94.0% after 5000 cycles at 5 A g−1. This study provides new insights into the surface‐defects dependent Zn deposition process and offers a guide for constructing stable surface for dendrite‐free Zn growth. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries are inherently safe, but the severe dendrite growth and corrosion reaction on zinc anodes greatly hinder their practical applications. Most of the strategies for zinc anode modification refer to the research of lithium metal anodes on surface regulation without considering the intrinsic mechanisms of zinc anode. Herein, we first point out that surface modification cannot permanently protect zinc anodes due to the unavoidable surface damage during the stripping process by solid–liquid conversion. A bulk‐phase reconstruction strategy is proposed to introduce abundant zincophilic sites both on the surface and inside the commercial zinc foils. The bulk‐phase reconstructed zinc foil anodes exhibit uniform surfaces with high zincophilicity even after deep stripping, significantly improving the resistance to dendrite growth and side reactions. Our proposed strategy suggests a promising direction for the development of dendrite‐free metal anodes for practical rechargeable batteries with high sustainability. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: The severe dendrite growth on zinc anode in alkaline electrolyte brings great challenge to the development of zinc‐based batteries. It is a simple and effective strategy to inhibit zinc dendrite formation by introducing additives into the electrolyte. In this study, N, S‐doped carbon dots (TU‐CQDs) were synthesized and used as additives to regulate zinc deposition in a typical KOH electrolyte. The experimental and three‐dimensional transient nucleation model disclosed that the special functional groups of carbon dots can change the electrode surface state and the coordination behaviors of zinc species in the electrolyte. Therefore, TU‐CQDs can not only inhibit the hydrogen evolution reaction, but also achieve uniform zinc deposition. The in‐situ synchrotron radiation X‐ray imaging elucidated that TU‐CQDs can effectively inhibit the dendrite growth and improve the reversibility of zinc plating/stripping process. This work provides a feasible route for regulating the reversibility of zinc metal anode in alkaline electrolyte. [ABSTRACT FROM AUTHOR]

The practical application of aqueous zinc batteries (AZBs) is significantly limited by the poor reversibility of the zinc anodes, including rampant dendrite growth and severe interfacial side‐reactions. Herein, trace hexamethylenetetramine (HMTA) additive with a lone‐pair‐electron containing heterocycle is introduced for Zn metal anode protection. Specifically, the trace added HMTA can change the solvated structure by strong interaction with zinc ions, and preferentially absorb on the anode surface to in situ establish an unique anode–molecule interface. Such an interface not only shows strong affinity to promote the dynamic transmission and deposition of Zn2+ ions but also displays a role in suppressing parasitic reactions. Consequently, a zinc anode in an electrolyte with trace HMTA achieves a high Coulombic efficiency of 99.75%, and delivers a remarkable lifespan over 4000 h at 5 mA cm−2 and 1 mAh cm−2 in a Zn//Zn symmetric cell. Even under a deep plating/stripping condition (5 mA cm−2 and 5 mAh cm−2), it can still run almost for 600 h. Additionally, the Zn//V2O5 full cell with HMTA retains a high capacity retention of 61.7% after 4000 cycles at 5 A g−1. Such an innovative strategy is expected to be of immediate benefit to design low‐cost AZBs with ultra‐long lifespan. [ABSTRACT FROM AUTHOR]

Developing a highly stable and dendrite‐free zinc anode is essential to the commercial application of zinc metal batteries. However, the understanding of zinc dendrites formation mechanism is still insufficient. Herein, for the first time, we discover that the interfacial heterogeneous deposition induced by lattice defects and epitaxial growth limited by residual stress are intrinsic and critical causes for zinc dendrite formation. Therefore, an annealing reconstruction strategy was proposed to eliminate lattice defects and stresses in zinc crystals, which achieve dense epitaxial electrodeposition of zinc anode. The as‐prepared annealed zinc anodes exhibit dendrite‐free morphology and enhanced electrochemical cycling stability. This work first proves that lattice defects and residual stresses are also very important factors for epitaxial electrodeposition of zinc in addition to crystal orientation, which can provide a new mechanism for future researches on zinc anode modification. [ABSTRACT FROM AUTHOR]

The most commonly used zinc foil anode for aqueous zinc‐ion batteries suffers from poor cycle stability and low zinc utilization. Zinc‐plated anodes on the host materials with high zincophilicity and stability are receiving increasing attention to alleviate these above issues. Here, the high zinc deposition activity of Cu (2 2 0) is confirmed through experimental observations and theoretical calculations and then Cu (2 2 0) substrates are prepared with the highly preferred orientation through an industrial electrolysis strategy. The prepared Cu (2 2 0) substrate can consistently modulate dense zinc growth by inducing the Zn (0 0 1) growth with the lowest surface energy and exposing high‐index zinc facets due to its exceptional grain size, high deposition activity, and homogeneous crystal orientation, which result in the high zinc plating/stripping reversibility of this Cu (2 2 0) substrate. When assembled into the Zn//MnO2 battery, the zinc‐plated Cu (2 2 0) can deliver capacity retention of 93.9% after 640 cycles at high zinc utilization (≈20%). This scalable orientation design strategy provides a new perspective for realizing dendrite‐free metal deposition with special textures. [ABSTRACT FROM AUTHOR]

Building an artificial interphase layer for tackling uncontrollable Zn dendrites and serious side reactions is a highly desirable strategy, but it is often hampered by the limited Zn2+ transport. Here, a stable fluorine‐doped amorphous carbon (CF) artificial layer is constructed on a Cu current collector (CF‐Cu) via facile carbonization treatment of a fluoropolymer coating to realize underlying Zn deposition. As evidenced experimentally and theoretically, this inorganic CF layer with ionic conductivity and electronic insulation successfully triggers dendrite‐free Zn deposition at the CF‐Cu interface with preferred Zn(002) crystal plane stacking parallel to the substrate surface, thus greatly promoting the inhibition of Zn‐dendrites and blocking of interfacial side reactions. The introduced fluorine atoms as abundant zincophilic sites play an important role in driving fast zinc‐ion transfer kinetics, which can partly convert into ZnF2 as an artificial solid Zn2+ conductor to further guide uniform Zn deposition. Consequently, the CF‐Cu electrode enables high reversibility with 99% coulombic efficiency and a long cycling stability of 1900 cycles at 2 mA cm–2. The integrated CF‐Cu@Zn anode achieves up to 2200 h cycles with a low voltage polarization. This study provides inspiration for the design of artificial interphase layers for stable nondendritic metal batteries. [ABSTRACT FROM AUTHOR]

The practical implementation of Zn metal anodes with high volumetric capacity is seriously plagued by the dendritic growth and accompanying interfacial parasitic reactions. Herein, high yield carbon dots (CDs) with abundant polar functional groups (CHO and CN), as a functional artificial interface layer, are rationally designed to optimize electrolyte/Zn interfaces with large‐scale viability. Of particular note, the quantum‐sized CDs with strong Zn affinity can effectively ameliorate the electric field distribution and ensure that more Zn2+ is adsorbed onto the whole electrode, which are beneficial for lowering the barrier of Zn2+ nucleation and inducing homogeneous Zn deposition, thus rendering a dendrite‐free Zn anode, as extensively confirmed by in situ optical microscope observation and finite element simulation. Meanwhile, the dense and insoluble coating layer with abundant polar functional groups is conducive to arousing the repulsion effect, which is good for shielding the active water and SO42−, thus eliminating the water‐mediated parasitic reactions and improving Zn2+ reaction kinetics. More importantly, the electrochemically stable CDs layer endows the Zn anode with a prolonged lifespan of 3000 h at 1 mA cm−2. This feasible and efficient fabrication of functional CDs layer opens a new avenue for stable dendrite‐free metal anodes. [ABSTRACT FROM AUTHOR]

Advanced materials with various micro‐/nanostructures have attracted plenty of attention in energy storage field over the past decades. Metallic reduction reactions (MRRs) possess the merits of low energy consumption, flexibility, convenience, and scalability, which have been considered as potential methods to acquire diverse micro‐/nanostructured materials. In this review, the latest progress of MRRs is systematically summed up, featuring the usage of metallic reductants (e.g., magnesium, aluminum, zinc, lithium) on synthesizing of advanced micro‐/nanostructured materials and their applications in various energy storage systems. The as‐obtained materials (e.g., carbon‐, silicon‐, germanium‐, antimony‐, and titanium‐based materials) can deliver various architectures, including solid spherical structures, hollow porous structures, core–shell structures, yolk–shell structures, core–satellite structures, and many kinds of 1D, 2D, 3D micro‐/nanostructures. Besides, the defect properties of materials can be well tuned via MRRs. The application progress of these materials as active electrodes, host materials, or functional interlayers for lithium ion batteries, lithium sulfur batteries, sodium ion batteries, or supercapacitors is reviewed. In the end, the strengths and insufficiencies of MRRs are discussed and the probable future research directions of MRRs are proposed. [ABSTRACT FROM AUTHOR]

Rechargeable aqueous zinc-ion batteries are a promising candidate for next-generation energy storage devices. However, their practical application is limited by the severe safety issue caused by uncontrollable dendrite growth on zinc anodes. Here we develop faceted titanium dioxide with relatively low zinc affinity, which can restrict dendrite formation and homogenize zinc deposition when served as the protective layer on zinc anodes. The as-prepared zinc anodes can be stripped and plated steadily for more than 460 h with low voltage hysteresis and flat voltage plateau in symmetric cells. This work reveals the key role of crystal orientation in zinc affinity and its internal mechanism is suitable for various crystal materials applied in the surface modification of other metal anodes such as lithium and sodium. Zinc affinity plays a key role in the zinc plating and stripping processes but its internal mechanism is still unclear. Here, the authors report a protective layer with controllable zinc affinity by adjusting the crystal orientation to suppress the dendrite growth on the zinc anode interface. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries have rapidly developed recently as promising energy storage devices in large‐scale energy storage systems owing to their low cost and high safety. Research on suppressing zinc dendrite growth has meanwhile attracted widespread attention to improve the lifespan and reversibility of batteries. Herein, design methods for dendrite‐free zinc anodes and their internal mechanisms are reviewed from the perspective of optimizing the host–zinc interface and the zinc–electrolyte interface. Furthermore, a design strategy is proposed to homogenize zinc deposition by regulating the interfacial electric field and ion distribution during zinc nucleation and growth. This Minireview can offer potential directions for the rational design of dendrite‐free zinc anodes employed in aqueous zinc‐ion batteries. [ABSTRACT FROM AUTHOR]

Rechargeable aqueous zinc‐ion batteries have been considered as a promising candidate for next‐generation batteries. However, the formation of zinc dendrites are the most severe problems limiting their practical applications. To develop stable zinc metal anodes, a synergistic method is presented that combines the Cu‐Zn solid solution interface on a copper mesh skeleton with good zinc affinity and a polyacrylamide electrolyte additive to modify the zinc anode, which can greatly reduce the overpotential of the zinc nucleation and increase the stability of zinc deposition. The as‐prepared zinc anodes show a dendrite‐free plating/stripping behavior over a wide range of current densities. The symmetric cell using this dendrite‐free anode can be cycled for more than 280 h with a very low voltage hysteresis (93.1 mV) at a discharge depth of 80 %. The high capacity retention and low polarization are also realized in Zn/MnO2 full cells. [ABSTRACT FROM AUTHOR]

Keywords: Crystal Defects; Dendrite; Epitaxial Growth; Residual Stress; Zinc Anode EN Crystal Defects Dendrite Epitaxial Growth Residual Stress Zinc Anode 1 1 1 04/05/23 20230411 NES 230411 B Residual stress b and lattice defects in commercial zinc anodes are essential factors for dendrite formation during zinc deposition as they lead to a heterogeneous deposition and limit the epitaxial growth of zinc. In their Research Article (e202218612), Haiyan Wang et al. propose an annealing strategy for lattice defect repair and residual stress relief. In their Research Article (e202218612), Haiyan Wang et al. propose an annealing strategy for lattice defect repair and residual stress relief. [Extracted from the article]

Dendritic inhibition is crucial for the cycle and reversibility of zinc‐based batteries. In this work, the trace metal ions including lead, copper, and nickel are used as additives to inhibit the growth of zinc dendrites. The interfacial evolution behaviors of zinc deposits during plating and striping processes are in situ observed by synchrotron radiation X‐ray imaging technique. The addition of lead and nickel ions induces a polarization role for zinc reduction, whereas copper ions present a depolarization role. After adding trace lead or nickel ions, zinc deposits become smoother and dendrites are effectively suppressed because of the homogenous deposition sites induced by co‐deposition of lead or nickel. Due to the depolarization role of copper ions, a large number of bubbles generate on the substrate and the loose zinc dendrites adhere on the bubble surface. In addition, the zinc deposits in the presence of trace lead ions present a more homogeneous stripping behavior. These results are helpful for understanding the inhibition role of metal ions additives on zinc dendrites and potentially improve the reversibility of zinc‐based batteries. [ABSTRACT FROM AUTHOR]

Titelbild: The Three-Dimensional Dendrite-Free Zinc Anode on a Copper Mesh with a Zinc-Oriented Polyacrylamide Electrolyte Additive (Angew. Wie H. Wang et al. in der Zuschrift auf S. 15988 ff. demonstrieren, kann die anfangs gebildete, feste Cu-Zn-Lösung die Zinkkeimbildung regulieren, während PAM das Wachstum von Zinkdendriten in den Folgezyklen unterdrückt. Wie H. Wang et al. in der Zuschrift auf S. 15988 ff. demonstrieren, kann die anfangs gebildete, feste Cu-Zn-Lösung die Zinkkeimbildung regulieren, während PAM das Wachstum von Zinkdendriten in den Folgezyklen unterdrückt. [Extracted from the article]

Comprehensive Summary: The severe dendrite growth on zinc anode in alkaline electrolyte brings great challenge to the development of zinc‐based batteries. It is a simple and effective strategy to inhibit zinc dendrite formation by introducing additives into the electrolyte. In this study, N, S‐doped carbon dots (TU‐CQDs) were synthesized and used as additives to regulate zinc deposition in a typical KOH electrolyte. The experimental and three‐dimensional transient nucleation model disclosed that the special functional groups of carbon dots can change the electrode surface state and the coordination behaviors of zinc species in the electrolyte. Therefore, TU‐CQDs can not only inhibit the hydrogen evolution reaction, but also achieve uniform zinc deposition. The in‐situ synchrotron radiation X‐ray imaging elucidated that TU‐CQDs can effectively inhibit the dendrite growth and improve the reversibility of zinc plating/stripping process. This work provides a feasible route for regulating the reversibility of zinc metal anode in alkaline electrolyte. [ABSTRACT FROM AUTHOR]

• A bifunctional layer was prepared in-situ on Zn metal anode. • The bifunctional layer can homogenize the electric field. • The epitaxial deposition of Zn (0 0 2) can be achieved. • The corrosion resistance of Zn anode has been improved. • Dendrite-free Zn plating/stripping is realized over 2200 h. Suppressing the Zn dendrites of the anode is regarded beneficial to constructing the high safe and long life Zn metal battery. However, it is still an austere challenge to realizing the even zinc nucleation and controllable growth. Herein, we reported a dendrite-free Zn anode based on the protection of Ag nanoparticles modified reduced graphene oxide (rGO/Ag@Zn). Among them, the parallelly aligned rGO layers drive the epitaxial deposition of Zn along (0 0 2) plane, while ultrafine Ag nanoparticles serve as the zincophilic seeds anchored on rGO to modulate uniform Zn-ion distribution and realize horizontally confined Zn deposition. Such synergistic effect restrains the growth of Zn dendrites, enabling an ultra-stable Zn anode. Therefore, the rGO/Ag@Zn symmetric cell can steadily cycle over 2200 h with a lower voltage polarization of 33.1 mV at a high current density and areal capacity (10 mA cm−2 and 5 mA cm−2). Meanwhile, the full cell matched with V 2 O 5 cathode delivers a high capacity of 157.5 mA h g−1 after 4000 cycles at 5 A/g. This bifunctional protection layer on Zn anode leads a dendrite-free Zn platting/stripping and provides a facile approach for high-performance zinc ion batteries. [ABSTRACT FROM AUTHOR]

[Display omitted] • Strong binding energy of sulfonated CDs toward Zn2+ could manipulate the Zn nucleation process. • Electrostatic repulsion between SO 4 2− and negative charge of CDs could mitigate formation of by-products. • Interfacial hydrogen bonds between CDs and water could restrain the water-induced side reaction. • Robust Zn-electrolyte interface with an ultra-durable lifespan of 4000 h at 1 mA cm−2 was successfully achieved. Water-induced side reactions and the growth of zinc dendrites are generally considered as the key problems hindering the development of zinc batteries. Herein, robust electrode/electrolyte interface is successfully constructed via introducing carbon dots (CDs) additive into hybrid electrolyte to enhance the stability of Zn anode. The CDs with -SO 3 − groups deliver strong binding energy toward Zn, which can reduce the nucleation barrier, thus favoring the homogeneous Zn deposition, as successfully evidenced by theoretical DFT calculation and intuitive in-situ optical microscope observation. Meanwhile, the zincophilic CDs can be preferentially adsorbed on the surface of Zn electrode, further diminishing water-induced adverse reaction by virtue of the electrostatic repulsion between SO 4 2− and negative charge of CDs. Accordingly, benefiting from the synergetic effect, the hybrid electrolyte with CDs endows Zn||Zn symmetric cell a prolonged lifespan over 4000 h with steady voltage fluctuation at 1 mA cm−2. [ABSTRACT FROM AUTHOR]

[Display omitted] • The DTBC-Zn anode was designed via an interfacial dissolution-coordination strategy. • The DTBC network improves the thermos-kinetics properties of Zn anode. • Zn2+ migrate along the coordination skeletons to achieve (0 0 2) plane deposition. • The DTBC-Zn anode enabled dendrite-free and by-product-free Zn deposition. Severe side reactions and dendrite growth are widespread in zinc anodes due to the aqueous electrolyte and the inhomogeneity of the Zn surface. Constructing an artificial interfacial layer on the zinc anode is a direct and effective strategy to solve these problems. Herein, a dithio-bridged chelate (DTBC) network consisting of zinc dimethyldithiocarbamate molecules was in situ constructed on the zinc surface via a facile interfacial dissolution-coordination strategy. The experiment and theoretical calculation revealed that the DTBC network simultaneously improves the thermos-kinetics properties of zinc anode. Moreover, the dithio groups in the DTBC network can induce the preferred plating of Zn along the (0 0 2) crystal plane and suppress dendrite growth. The DTBC-Zn electrode delivered an extended lifetime of over 1200 h with an ultralow polarization of ∼27.3 mV at 0.5 mA cm−2. The capacity retention rate of DTBC-Zn|MnO 2 full cell was as high as 97.98 % after 1600 cycles, further confirming the feasibility of the robust dithio-bridged chelate network for stabilizing thermo-kinetics of zinc anode. This work contributes a simple and effective way to construct high-performance zinc anodes for aqueous zinc ion batteries. [ABSTRACT FROM AUTHOR]

Zinc(II) was recovered from dilute ammoniacal media through an integrated process combining solvent extraction and electrolysis with ammonia stripping. Zinc ions were firstly enriched into organic phase at pH 7.56 through synergistic extraction between β-diketone and TBP or Cyanex 923. The concentration of extracted zinc(II) increased at pH < 7.56, but clearly decreased at pH 7.56–9.98. The extracted zinc species could be effectively stripped from the loaded organic phase using ammoniacal liquor at pH 9.5, because the ammonia stripping process followed an trend opposite to the extraction process. The extraction and ammonia stripping isotherms verified that Zn(II) concentration can be increased from 1.3 g/L to >56 g/L by using β-diketone and Cyanex 923. Metallic zinc can be obtained by direct electrolysis from the ammoniacal stripping solution. The presence of small amounts of the dissolved extractant molecules can improve the crystallization of zinc deposits. A gelatin additive was used to smoothen the morphology of zinc deposits and refine their crystalline structure. These results indicate that the proposed integrated process will facilitate the recovery of various zinc-bearing primary and secondary resources in ammoniacal media. • An integrated process was firstly proposed to recover zinc(II) from ammoniacal media. • Extraction and stripping processes of zinc present a special swing phenomenon. • Zn(II) is directly enriched from 1.3 g/L to 56 g/L by ammonia stripping. • Metal zinc can be obtained by direct electrolysis from ammonia stripping solution. • The dissolved extractant molecules can improve the crystallization of zinc deposits. [ABSTRACT FROM AUTHOR]