Bulk‐Phase Reconstruction Enables Robust Zinc Metal Anodes for Aqueous Zinc‐Ion Batteries

Yang, Zefang; Hu, Chao; Zhang, Qi; Wu, Tingqing; Xie, Chengzhi; Wang, Hao; Tang, Yougen; Ji, Xiaobo; Wang, Haiyan

doi:10.1002/anie.202308017

Cited by 24 publications

(19 citation statements)

References 42 publications

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“…The EDS mapping in the selected region indicates the deposition layer mainly comprising Zn, O, C, and Cl elements with homogeneous distribution. To accurately elucidate the structure and composition of the interphase, the eutectic‐assisted fabrication of SEI was witnessed by focused ion beam‐transmission electron microscope (FIB‐TEM) [24] . A lamella (10×3 μm) was milled by FIB from zinc foil in HZAH‐1 after 50 cycles at 0.5 mA cm −2 (Figure 5d, Figure S22, Figure S23).…”

Section: Resultsmentioning

confidence: 99%

Competitive Coordination Structure Regulation in Deep Eutectic Electrolyte for Stable Zinc Batteries

Deng,

Chen

et al. 2024

Angew Chem Int Ed

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Rechargeable zinc‐based batteries are finding their niche in energy storage applications where cost, safety, scalability matter, yet they are plagued by rapid performance degradation due to the lack of suitable electrolytes to stabilize Zn anode. Herein, we report a competitive coordination structure to form unique quaternary hydrated eutectic electrolyte with ligand‐cation‐anion cluster. Unraveled by experiment and calculation results, the competing component can enter initial primary coordination shell of Zn2+ ion, partially substituting Lewis basic eutectic ligands and reinforcing cation‐anion interaction. The hydration‐deficient complexes induced between competing eutectic as hydrogen bond donor‐accepter and water also broaden the electrochemical window and confine free water activity. The altered coordination further leads to robust hybrid organic‐inorganic enriched solid electrolyte interphase, enabling passivated surface and suppressed dendrite growth. Noticeably, stable Zn plating/stripping for 8000 cycles with high Coulombic efficiencies of 99.6% and long cycling life of 10000 cycles for Zn‐organic batteries are obtained. Even under harsh conditions (small N/P ratio, low temperature), the profits brought by the competitive eutectic electrolyte are still very prominent. This design principle leveraged by eutectic electrolytes with competitive coordination offers a new approach to improve battery performance.

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Section: Resultsmentioning

confidence: 99%

Competitive Coordination Structure Regulation in Deep Eutectic Electrolyte for Stable Zinc Batteries

Deng,

Chen

et al. 2024

Angew Chem Int Ed

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“…Electrochemical energy storage systems that are economical, secure, and ecologically benign are crucial for the efficient utilization of renewable energy. Owing to the non-toxic and inflammable properties of aqueous electrolytes, aqueous batteries are among the best options for low-cost, large-scale energy storage applications., [1][2][3][4][5][6] Among the variety of promising aqueous battery systems (Li + , [7,8] Na + , [9,10] K + , [11,12] Ca 2 + , [13] Mg 2 + , [14] Zn 2 + , [15][16][17][18][19] NH 4 + , [20,21] etc. ), aqueous zinc ion batteries (ZIBs) have received a lot of interest in recent years benefiting from high specific capacities of the zinc metal anode (820 mAh g À 1 and 5845 mAh cm À 3 ), relatively low potential (À 0.763 V vs. SHE, in mild or acidic electrolytes) and low cost.…”

Section: Introductionmentioning

confidence: 99%

Maximizing Electrostatic Polarity of Non‐Sacrificial Electrolyte Additives Enables Stable Zinc‐Metal Anodes for Aqueous Batteries

Zhou

Yang

et al. 2023

Angew Chem Int Ed

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Although additives are widely used in aqueous electrolytes to inhibit the formation of dendrites and hydrogen evolution reactions on Zn anodes, there is a lack of rational design principles and systematic mechanistic studies on how to select a suitable additive to regulate reversible Zn plating/stripping chemistry. Here, using saccharides as the representatives, we reveal that the electrostatic polarity of non‐sacrificial additives is a critical descriptor for their ability to stabilize Zn anodes. Non‐sacrificial additives are found to continuously modulate the solvation structure of Zn ions and form a molecular adsorption layer (MAL) for uniform Zn deposition, avoiding the thick solid electrolyte interphase layer due to the decomposition of sacrificial additives. A high electrostatic polarity renders sucrose the best hydrated Zn2+ desolvation ability and facilitates the MAL formation, resulting in the best cycling stability with a long‐term reversible plating/stripping cycle life of thousands of hours. This study provides theoretical guidance for the screening of optimal additives for high‐performance ZIBs.

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“…[34,35] Moreover, prolonged cycling of the Zn deposition/striping process may cause detachment and exfoliation of the polymer coatings, further compromising the long-term stability. [36,37] Therefore, the development of selfadapting polymer interface with well-bonded interfaces is highly desired to dynamically guarantee interface/electrode compatibility, which is crucial for achieving the durable, uniform and reversible Zn deposition. So far, such strategies have been rarely reported due to the challenges associated with in situ dynamic integration with Zn electrode.…”

Section: Introductionmentioning

confidence: 99%

In Situ Electrochemically‐Bonded Self‐Adapting Polymeric Interface for Durable Aqueous Zinc Ion Batteries

Zhang,

Deng

et al. 2023

Adv Funct Materials

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The implementation of aqueous zinc ion batteries (AZBs) is hindered by the notorious Zn dendrite growth and side reactions on Zn anodes. Herein, a novel strategy is introduced to overcome these hurdles by designing a self‐adapting soft polymeric composite interface (SAP). Unlike conventional methods relying on passive coating process, the approach leverages dynamic in situ electrochemical bonding via Zn─O interactions formed during cycling, ensuring intimate contact between the SAP interface and Zn electrode. The SAP interface boasts a robust network of hydrogen bonding and electrostatic interactions, which not only promotes the desolvation of Zn2+ and the repulsion of SO42−, facilitating uniform and rapid Zn2+ migration while effectively suppressing parasitic reactions; but also exhibits remarkable self‐adapting and self‐healing capabilities, enabling the interface to accommodate volume changes and repair mechanical failures over prolonged cycling. Consequently, highly reversible Zn electrodes are achieved with SAP, showcasing 3300 h at 1 mA cm−2/0.5 mAh cm−2 and 350 h at 20 mA cm−2/10 mAh cm−2 in the symmetric cells. The advantages of the SAP interface are further verified when paired with high mass loading LiMn2O4 cathodes in AZBs. The versatile SAP interface offers insights into advanced interface design for efficient and durable AZBs.

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Bulk‐Phase Reconstruction Enables Robust Zinc Metal Anodes for Aqueous Zinc‐Ion Batteries

Cited by 24 publications

References 42 publications

Competitive Coordination Structure Regulation in Deep Eutectic Electrolyte for Stable Zinc Batteries

Competitive Coordination Structure Regulation in Deep Eutectic Electrolyte for Stable Zinc Batteries

Maximizing Electrostatic Polarity of Non‐Sacrificial Electrolyte Additives Enables Stable Zinc‐Metal Anodes for Aqueous Batteries

In Situ Electrochemically‐Bonded Self‐Adapting Polymeric Interface for Durable Aqueous Zinc Ion Batteries

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