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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Ionic liquid-integrated aqueous electrolyte regulation on solvation chemistry and electrode interface for reversible dendrite-free zinc anodes

Hui-Juan Guo,Xiao-Jiang Chen,Rui Shu,Xiao-Bin Zhong,Li-Xin Zhang,Yue-Xian Song

Zn anodes suffer from poor reversibility and stability owing to nonuniform dendrite growth and self-corrosion. Here, 1-ethyl-3-methylimidazolium acetate (EMImAc) is introduced to reconstruct interfacial electrical double layer with simultaneously manipulating the solvation environment and the adsorption situation on Zn anode. The acetate anions with high nucleophilicity can effectively alter the solvation shell around Zn 2+ ions and immobilize the H 2 O molecules, thus weakening water activity and alleviating water-related parasitic reactions. Concomitantly, both the imidazolium cation and acetate anion are inclined to gather on Zn anode surface for constructing an electrostatic shielding layer, and meanwhile the chemisorbed acetate anions also contribute to accelerate the Zn(H 2 O) 6 2+ desolvation process. Such a synergistic effect enables uniform electric field distribution and facilitates Zn ion flux, which mitigates the random diffusion of Zn 2+ and finally promotes the dendrite-free deposition. As a result, the Zn/Zn symmetric cells with EMImAc-integrated aqueous electrolyte realize an excellent cycling lifespan of 7000 h (0.5 mA cm −2 /0.25 mAh cm −2 ) and high Zn utilization of 61.3 % (15 mA cm −2 /20 mAh cm −2 ). Furthermore, the effective of EMImAc additive is demonstrated in Zn/V 2 O 5 cells. This work offers insights into the ionic liquid-integrated aqueous electrolytes to enhance the interface stability of Zn anode for rechargeable zinc batteries.

研究领域: 材料科学 · 电化学
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Chemistry-An Asian Journal · 2021 ·Vol. 16 ·期 15 ·2146-2153 · IF 4.568

A ZIF-8 Host for Dendrite-Free Zinc Anodes and N,O Dual-doped Carbon Cathodes for High-Performance Zinc-Ion Hybrid Capacitors

Liling Lei,Yiwei Zheng,Xichen Zhang,Yutian Su,Xi Zhou,Shishan Wu,Jian Shen

Graphical A new zinc-ion hybrid capacitor assembled by using a Zn@annealed ZIF-8 anode and ZIF-8 derived C cathode provides a capacity of 135.5 mAh g −1 and an energy density of 108.4 Wh kg −1 with a power density of 800 W kg −1 at 1.0 A g −1 . Zn is a promising anode for aqueous energy storage owing to it intrinsic superior properties such as large capacity, abundant reserves, low potential and safety. But, the growth of dendrites during charge and discharge leads to a decrease in reversibility. In addition, further development of zinc-ion hybrid capacitors (ZICs) is seriously challenging because of the lack of an exceptional cathode. Herein, we use ZIF-8 annealed at 500 °C (annealed ZIF-8) as a host material for stable and dendrite-free Zn anodes. Utilization of annealed ZIF-8 results in dendrite-free Zn deposition and stripping as a result of its porous construction, which contains trace Zn. Furthermore, we firstly proposed innovative N,O dual-doped carbon which was designed by the derived ZIF-8 (ZIF-8 derived C) as cathode for high-energy and power-density ZICs. The new ZIC assembled by Zn@annealed ZIF-8 anode and ZIF-8 derived C cathode provides a capacity of 135.5 mAh g −1 and an energy density of 108.4 Wh kg −1 with a power density of 800 W kg −1 at 1.0 A g −1 . In addition, it shows outstanding cycling stability of 91% capacity retention after 6000 cycles at 5.0 A g −1 . Moreover, the solid-state ZICs can drive LEDs and smart watches. This ZIC holds promise for the practical application of supercapacitors.

研究领域: 材料科学 · 电化学 · 能源存储
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Journal of Energy Storage · 2025 · IF 9.8

3D tin whisker network enabling high-performance aqueous dendrite-free zinc anodes

Peigen Zhang,Tianyu Wang,Pei Ding,Feiyue Hu,Zhenglin Zou,Wei He,Vamsi Borra,Qinning Gao,Hanning Zhang,Jingwen Tang,Wei Zheng,ZhengMing Sun

Aqueous zinc-ion batteries (AZIBs) offer high safety, low cost, and environmental compatibility, yet their large-scale deployment is hindered by dendrite growth and severe side reactions arising from non-uniform Zn 2+ deposition. Constructing artificial interphase layers (AILs) to regulate Zn 2+ nucleation and growth has emerged as an effective strategy to mitigate these issues. One-dimensional (1D) Sn metal, featuring a high specific surface area, tunable structure, strong zinc affinity, and high hydrogen evolution overpotential, is an ideal candidate for interphase engineering. However, existing synthesis methods for 1D Sn, which rely on template-assisted electrodeposition, face challenges in scalability. In this work, Sn whiskers are synthesized via the mechanochemical decomposition of the Ti 2 SnC MAX phase and employed to construct a three-dimensional (3D) Sn whisker network as an artificial interphase layer on zinc anodes (Sn whisker@Zn). This continuous network effectively guides Zn 2+ migration and deposition, promotes preferential growth along the (002) crystal plane, reduces local current density, and suppresses dendrite formation. Simultaneously, it retards corrosion and inhibits the formation of by-products. Symmetric cells based on Sn whisker@Zn anodes exhibit exceptional cycling stability, sustaining over 1600 h of stable operation at 1 mA cm −2 with a capacity of 0.5 mAh cm −2 , and exceeding 1000 h at a high current density of 10 mA cm −2 . Moreover, the Sn whisker@Zn||NH 4 V 4 O 10 full cell retains 89.94 % of its capacity after 1400 cycles at 5 A g −1 , demonstrating strong application potential. This approach provides a scalable and effective strategy for developing durable zinc anodes, advancing the prospects of AZIBs in energy storage systems.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 金属腐蚀与防护
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

In situ growth of S-doped ZnO thin film enabling dendrite-free zinc anode for high-performance aqueous zinc-ion batteries

Denglei Zhu,Yufan Zheng,Yi Xiong,Chaojun Cui,Fengzhang Ren,Yong Liu

Aqueous rechargeable zinc-ion batteries (AZIBs) have gained extensive attentions due to their high volumetric capacity, low cost, and intrinsic safety. Nonetheless, their zinc metal anodes have been suffered from many issues, such as uncontrollable dendrite growth and undesired side reactions, which eventually degrade the capacity and cycle life. Herein, a thin sulfur-doped zinc oxide artificial interface film (≈200 nm) was in situ grown on zinc foil (ZnO:S@Zn) by a simple chemical bath deposition method. The density functional theory calculations revealed that the electronic conductivity of zinc oxide could be improved after sulfur doping. Characterization analyses and electrochemical measurements showed that this unique film could enhance the electrical conductivity of zinc anode inhibit the side reaction and induce Zn 2+ uniform deposition. As a result, the ZnO:S@Zn symmetric cell was stably cycled for 1700 h at 0.5 mA cm −2 with a stable voltage hysteresis of ~20 mV, and the full-cell pairing with MnO 2 cathode exhibited an excellent reversible capacity of 297.46 mAh g −1 after 300 cycles. This work offers a simple and effective way to fabricate a stable Zn metal anode for high performance AZIBs.

研究领域: 材料科学 · 电化学 · 能源存储
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Two-pronged approach to achieving high-capacity and long stable-life aqueous Zn-ion batteries

Huaqing Chen,Yuyan Wang,Shujia Zhang,Yuting He,Linrui Hou,Changzhou Yuan

Rechargeable Zn-ion batteries (ZIBs) have attracted much attention due to their high energy density, high safety, and low cost. Nevertheless, the practical implementation of ZIBs has been dreadfully hindered by the lack of stable high-capacity cathode candidate and serious dendritic growth in Zn anode. Superior device-level performance can only be achieved by simultaneously addressing the fatal shortcomings of both electrodes. Herein, we explore a two-pronged approach to achieving high-capacity, long-life stable ZIBs via synergistic design in both anodes and cathodes. Specifically, hierarchical accordion-like ZnV 2 O 4 @C (A-ZVO@C) framework derived from multi-layered V 2 CT x is fabricated and endowed with high electronic/ionic conductivities and structural/chemical stability, exhibiting striking high-rate capacities/stability when utilized as a cathode. Meanwhile, a dendrite-free Zn with an artificial protective layer of zincophilic ZnO/C hollow spheres affords outstanding Zn plating-stripping stability with a prolonged lifespan, which reduces local current density, homogenizes Zn 2+ ion diffusion/deposition, and suppresses volume changes during long-term plating/stripping. As a result, the assembled full ZIBs deliver a high-rate capacity of 232.2 mAh g −1 at 8 A g −1 , and superb stability with capacity degradation of 7.8 % over 3000 consecutive cycles at 15.0 A g −1 . More meaningfully, the contribution here provides an essential guidance for rationally designing next-generation ZIBs.

研究领域: 能量存储 · 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Simultaneous regulation on solvation shell and electrode interface for sustainable zinc-based flow batteries

Tao Xuan,Xusheng Cheng,Liwei Wang

The practical implementation of Zn-based flow batteries encounters the challenges associated with uneven deposition of Zn ions and undesirable side reactions. Here, a hybrid Zn-based electrolyte system composed of ZnBr 2 , ethylene glycol (EG), H 2 O and potassium gluconate (KGlu) is developed as anolyte to modulate the solvation structure and interface engineering for a sustainable Zn-based flow battery. The EG molecules could exclude water molecules outside the solvation structure, inhibiting the water-induced side reactions and Zn corrosion. Moreover, the incorporation of potassium gluconate constructs an artificial stable anionic interface for dendrite-free Zn deposition. Chemical stability and hydrogen evolution potential tests demonstrate that the activity of water molecules could be suppressed in the EG-containing hybrid electrolyte. Deposition morphologies and Zn//Zn symmetric flow battery tests also reveal that gluconate anions preferentially adsorbed on zinc anode could effectively facilitate uniform zinc deposition. As a result, the Zn-based flow battery with the proposed hybrid electrolyte delivers a stable cycling performance over 200 cycles and high reversibility with an average CE of over 97.4 % at 20 mA cm −2 , exhibiting a peak power density of 103.2 mW cm −2 . This work provides a universal electrolyte design strategy for realizing a sustainable Zn-based flow battery.

CAS / MDL: 107-21-1 7699-45-8
研究领域: 储能技术 · 电化学 · 材料科学
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Nature Communications · 2025 · IF 15.7

Gradient chaotropic regulation of Zn2+ solvation chemistry for low-temperature zinc metal batteries

Yang Sinian,Zhao Shunshun,Xu Haojie,Wang Xinwei,Huang Xuanrui,Yang Qi,Chen Yong,Wang Guoxiu,Chen Shimou

Aqueous zinc-ion batteries have emerged as a promising system for safe and sustainable energy storage. However, their practical application is hindered by detrimental interfacial side reactions and inadequate low-temperature performance. Herein, we report the design of a gradient chaotropic ionic liquid (IL)-based aqueous electrolyte (Emim⁺-TFA⁻/OTf⁻-Zn 2+ -H 2 O), which can simultaneously fulfil the conflicting demands of dendrite-free zinc deposition and low-temperature operation. By forming an antifreeze electrolyte with a hydrophobic yet salt-philic interface, the proposed formulation overcomes the limitations of conventional IL-based systems that rely on H 2 O-lean compositions, complex additives, or elaborate solvent mixtures. Thus, the assembled zinc-ion cells exhibit improved zinc plating/stripping stability. At a current density of 0.1 mA cm −2 and 0.1 mAh cm −2 , the Zn | |Zn symmetric cells endure prolonged zinc plating/stripping, exceeding 13,000 h at −30 °C and 6690 h at −40 °C. In full cells, Zn | |VO 2 @VO maintains nearly 100% capacity retention over 3500 cycles at 0.2 A g −1 and −40 °C. This gradient chaotropic Zn 2+ electrolyte design provides a versatile platform for effective antifreeze Zn 2+ solvation chemistry and accelerated interfacial ion transport, enabling high-performance zinc batteries in subzero environments.

CAS / MDL: 1314-62-1 872-50-4
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Electrolyte-Tailored Heterostructured Zinc Metal Anodes with Tunable Electric Double Layer for Fast-Cycling Aqueous Zinc Batteries

Jingteng Zhao,Shaobo Ma,Zhongqiang Wang,Qixin Gao,Huang Xiao,Jian Gao,Fang Li,Guoxing Li

The structures and properties of the electric double layer (EDL) on zinc (Zn) anodes significantly influence the cycling and rate performance of aqueous Zn batteries (ZBs). Here, a strategy is reported to regulate the EDL structure through work function ( W f ) engineering to effectively enhance the electrochemical performance of ZBs, which is enabled by electrolyte-tailored growth of heterogenous metal with a large W f on the Zn anode. The metal-to-metal charge transfer in heterostructured Zn metal induced by the disparity of W f increases the surface charge density, which enriches the Zn ions and shortens the thickness of EDL. The compressed EDL weakens the repulsive force of Zn deposits to achieve a tightly stacked and dendrite-free Zn deposition. Besides, the formed H 2 O-deficient EDL structure enables the inorganic-rich solid electrolyte interphase (SEI) with high Zn-ion conductivity to inhibit the notorious parasitic reactions and improve the electrode reaction kinetics. Consequently, the Zn||Zn symmetric cells demonstrate an ultra-long cycling life over 2700 cycles (the cumulative capacity reaches 5400 mA h cm −2 ) at a high current density of 50 mA cm −2 . The Zn anodes show a high average Coulombic efficiency of 99.70% over 3650 cycles. The Zn||MnO 2 full cells exhibit excellent practical-level performance under cyclic continuous mode (3000-cycle life at high rates) and cyclic intermittent mode (1170-cycle life with 83.05% capacity retention). Practical pouch cells are also demonstrated with outstanding cycling performance.

研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

Fast anion intercalation into graphite cathode enabling high-rate rechargeable zinc batteries

Zheng Chen,Tianmeng Liu,Zhiming Zhao,Zhonghua Zhang,Xiaoqi Han,Pengxian Han,Jiedong Li,Jinzhi Wang,Jiajia Li,Suqi Huang,Xinhong Zhou,Jingwen Zhao,Guanglei Cui

Cheap, high-rate and long-life batteries are urgently needed for grid-scale storage of renewable energy. Rechargeable zinc (Zn) batteries are potential candidates due to the high volumetric energy density and low cost of Zn anode. However, conventional Zn batteries employing metal oxide cathodes usually suffer from poor rate capabilities caused by the high migration barrier of Zn 2+ in the metal oxide host structure. Here, we circumvent this dilemma by integrating Zn electrochemistry with bis(trifluoromethanesulfonyl) imide (TFSI − ) anion (de)intercalation into graphite cathode based on a Zn(TFSI) 2 /acetonitrile electrolyte. Owing to the fast intercalation of TFSI − along with the efficient Zn/Zn 2+ redox kinetics, our Zn/graphite batteries enable an ultrafast charging rate up to 200C (to be fully charged in 18 s) and deliver a high power density of 16.3 kW kg −1 , which is comparable to those of supercapacitors . Besides, the rational utilization of the acetonitrile-based electrolyte further endows the resultant battery with dendrite-free Zn deposition, high voltage output (>2.2 V) as well as wide-temperature adaptability from −40 to 80 °C, which is quite promising for grid-scale energy storage. Our work opens a new avenue for building high-rate low-cost batteries through coupling anion intercalation chemistry with multivalent metal anodes.

CAS / MDL: 872-50-4
研究领域: 能源存储 · 电池技术 · 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Sieve-Like interface built by ZnO porous sheets towards stable zinc anodes

Yujun Zhou,Shiyin Xie,Yang Li,Zhiyuan Zheng,Liubing Dong

Zn-based electrochemical energy storage (EES) systems are plagued by the uncontrollable generation of dendritic zinc and side reactions on zinc anodes. Herein, we report a ZnO porous sheets-assembled sieve-like interface to stabilize zinc anodes. Specifically, ZnO porous sheets are synthesized through the thermal decomposition of basic zinc sulfate nanoflakes and then served as an artificial zinc anode-electrolyte interface. Benefiting from the sieve-like interface formed by the ZnO porous sheets, Zn 2+ flux is effectively homogenized during the zinc plating process and thus zinc dendrite growth is restricted. Meanwhile, the corrosion behavior of zinc anodes is alleviated thanks to the hydrophobic feature of the ZnO porous sheets. As a result, the electrochemical properties of zinc anodes are notably optimized under the protection of such a sieve-like interface. Cycling life evaluated at 1 mA cm −2 of the zinc anodes is prolonged from less than 100 h for bare zinc anodes to 2800 h for the protected zinc anodes (Zn@ZnO), and even at 5 mA cm −2 , the latter ones can operate normally for 400 h. As expected, the cycling life of VO 2 //Zn@ZnO zinc-ion batteries is greatly increased, achieving 90% capacity retention after 1000 cycles at 5 A g −1 and activated carbon fiber//Zn@ZnO zinc-ion hybrid supercapacitors possess 96% capacity retention after 10,000 cycles at 1 A g −1 . This work provides a promising approach for improving the electrochemical stability of the Zn-based EES system.

研究领域: 电化学 · 材料科学 · 能源存储
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ACS Nano · 2022 · IF 18.027

A Functional Organic Zinc-Chelate Formation with Nanoscaled Granular Structure Enabling Long-Term and Dendrite-Free Zn Anodes

Huaming Yu,Yuejiao Chen,Weifeng Wei,Xiaobo Ji,Libao Chen

Aqueous Zn metal batteries suffer from rapid cycling deterioration due to the severe water corrosion and dendrite growth on Zn anodes. Herein, a highly antiwater Znx-diethylenetriaminepenta(methylene-phosphonic acid) interface layer with good zinc affinity and special nanoscaled 3D granular structure is designed on Zn metal to address these problems. Experimental results combined with theoretical analysis and COMSOL simulations reveal that the hydrophobic groups in such Zn-based organic complex are the decisive factor in preventing H2O from damaging Zn anode surface. The massive Zn2+ attractive sites formed by interaction of methylene-phosphonic acid groups and Zn cause ion channel for fast zinc-ion adsorption and migration. And the developed nano granular architecture on the surface induces redistributed Zn2+ ion flux to realize homogenization with smooth and compact surface deposition. Under the synergism, such modified anodes exhibit long cycling lifespan over 1300 h with a relatively low polarization voltage at 5 mA cm–2. Also, the assembled full cells (including Zn//V2O5 and Zn//MnO2 cell) based on this anode are also demonstrated. The work provides a simple, low cost, and efficient pathway by combining the two concepts of structural design and constructing protective layers on the surface to prepare high-performance Zn anodes toward prospering aqueous zinc–metal batteries.

CAS / MDL: 1314-62-1
研究领域: 材料科学 · 电化学 · 电池技术 · 纳米技术
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