Functionalizing the interfacial double layer to enable uniform zinc deposition

Li, Yihu; Wang, Hao; Wu, Tingqing; Xie, Chunlin; Yang, Zefang; Zhang, Qi; Sun, Dan; Tang, Yougen; Wang, Haiyan

doi:10.1007/s11426-022-1590-y

Cited by 5 publications

(1 citation statement)

References 44 publications

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“…Inspired by the illustration in Figure a, the eutectic-induced Helmholtz EDL can be compared to the EDL of conventional aqueous electrolytes, as shown in Figure b, where the metal electrodes (taking the Zn anode as examples) are negatively charged during electrodeposition, delivering an initial potential of ψ 0 and positive metal ions (e.g., Zn 2+ cations) are absorbed. Accordingly, the deposition potential of the Zn surface immersed in the conventional aqueous electrolyte increases from ψ 0 to ψ ξ . However, the eutectic constitution (via Lewis acid–base and H-bonding interactions) assists in the reconstruction of the IHP near the Zn surface due to the high affinity of eutectic–solvating Zn 2+ coordination structures, excluding the presence of free-water but allowing the eutectic–H 2 O complex structure to participate in the OHP and diffusion layer and presenting a higher potential ψ′ ξ than ψ ξ …”

Section: Eutectic Thermodynamics and Mass Transportmentioning

confidence: 99%

Eutectic Electrolytes Convoying Low-Temperature Metal-Ion Batteries

Qu,

Lu,

Jiang

et al. 2024

ACS Energy Lett.

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Eutectic electrolytes have been widely used in low-temperature metal-ion batteries (MIBs) due to their good performance regardless of seasonal and regional changes. Durable low-temperature MIBs rely on the constitution, proportion, and solvation-structure construction of eutectic electrolytes to maintain high ionic conductivity and electrochemical stability. Despite the rapid advances in eutectic electrolytes, some key issues, including fundamental mechanisms, theoretical models, aqueous/non-aqueous controversies, and challenges at sub-zero temperatures, need to be addressed. This Review first gives an overview of eutectic chemistry by presenting fundamental analysis and proposing new models to demonstrate the variety of interactions and anti-freezing mechanisms. Then, the thermodynamics and mass transfer, Helmholtz electric double-layer configuration, and electrode–electrolyte interphase are discussed to uncover the influence of the eutectic structure on the electrochemistry of low-temperature MIBs. Finally, a summary and perspectives are provided to guide the design principles and requirements of eutectic systems for applications of MIBs in low-temperature scenarios.

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Section: Eutectic Thermodynamics and Mass Transportmentioning

confidence: 99%

Eutectic Electrolytes Convoying Low-Temperature Metal-Ion Batteries

Qu,

Lu,

Jiang

et al. 2024

ACS Energy Lett.

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Helmholtz Plane Reconfiguration Enables Robust Zinc Metal Anode in Aqueous Zinc‐Ion Batteries

Wu,

Hu,

Zhang

et al. 2024

Adv Funct Materials

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Aqueous zinc‐ion batteries are promising for next‐generation energy storage systems. However, the zinc dendrite growth, corrosion, and hydrogen evolution reaction at the electrochemical interface severely impede their further development. Herein, a Zn2+‐rich and H2O‐poor Helmholtz plane is constructed to regulate the electrochemical interface between the zinc anode and the electrolyte. Electrochemical and in situ spectroscopy characterizations reveal that the designed electric double layer with abundant Zn2+ coordination sites and less H2O content can facilitate rapid electron transfer, homogenize Zn2+ deposition, and alleviate the side reactions induced by active H2O. Benefiting from the high reversibility and stability of zinc anode, the Zn||Zn symmetric cell can be cycled over 1000 h at 1 mA cm−2 and the Zn||NH4V4O10 full cell can maintain a capacity of 85.23% for 1000 cycles at 3 A g−1. This work aims at Helmholtz plane reconfiguration and provides a realizable strategy in interface construction for other similar systems.

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Zwitterionic Organic Multifunctional Additive Stabilizes Electrodes for Reversible Aqueous Zn‐Ion Batteries

Zhang,

Liu,

Wang

et al. 2024

Adv Funct Materials

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Aqueous zinc‐ion batteries (AZIBs) exhibit significant potential for grid energy storage due to their low cost and safety. However, the commercial applications of AZIBs face challenges, particularly in the anode, such as zinc dendrites, hydrogen evolution reaction (HER), and zinc corrosion. In this study, a protonated triglycine (ggg) as a multifunctional electrolyte additive for AZIBs is employed. This ggg molecule can dissociate as zwitterion (both anion and cation) in mildly acidic ZnSO4 electrolytes. The NH3+ cation in ggg molecule can adsorb on the surface of the zinc anode, regulating the deposition of Zn2+ and slowing down the side reactions, and the spontaneously dissociated ggg anions will combine with Zn2+ to regulate the solvated Zn2+ chemistry in the electrolyte, establishing the electrostatic interaction via the strong adsorption ability to Zn2+. Theoretical calculations indicate that ggg molecule demonstrates a strong affinity toward Zn2+, enabling the reconstruction of Zn(H2O)62+ and facilitating subsequent de‐solvation processes. As a result, Zn||Zn symmetric cells in ZnSO4/0.2 mM ggg electrolyte exhibited an extended cycling lifetime of ≈4500 h. Furthermore, the Zn||MnO2 full battery demonstrated enhanced capacity and cycling performance with the addition of ggg molecule. This study provides valuable insights into constructing a highly reversible electrolyte for AZIBs.

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Functionalizing the interfacial double layer to enable uniform zinc deposition

Cited by 5 publications

References 44 publications

Eutectic Electrolytes Convoying Low-Temperature Metal-Ion Batteries

Eutectic Electrolytes Convoying Low-Temperature Metal-Ion Batteries

Helmholtz Plane Reconfiguration Enables Robust Zinc Metal Anode in Aqueous Zinc‐Ion Batteries

Zwitterionic Organic Multifunctional Additive Stabilizes Electrodes for Reversible Aqueous Zn‐Ion Batteries

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