2-methyl imidazole electrolyte additive enabling ultra-stable Zn anode

Wu, Changcai; Sun, Chuang; Ren, Kaixin; Yang, Feng; Du, Yixun; Gu, Xiaosi; Wang, Qinghong; Lai, Chao

doi:10.1016/j.cej.2022.139465

Cited by 56 publications

(30 citation statements)

References 37 publications

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“…In addition, a prolonged lifespan of 1500 h was also achieved at a high current density of 5 mA cm –2 for the KevlarH electrolyte (Figure S8). Besides, the KevlarH electrolyte also delivered an impressive CE improvement (99.87%) over 2500 cycles (Figure b), which is superior to most, if not all, recently reported electrolyte regulation studies for Zn metal anodes (Figure c). ,− Inspired by the exceptional Zn deposition/stripping reversibility and interface stability with the KevlarH electrolyte, Zn||V 2 O 5 full batteries were fabricated to probe its feasibility in full cells. As shown in Figures d and S9, the Zn||V 2 O 5 full cell using a thin Zn foil (thickness of 20 μm) with a limited N/P ratio of 4.3 in the KevlarH electrolyte exhibited a high areal capacity of ∼1.2 mAh cm –2 after 1500 cycles at 5 A g –1 with good interfacial stability (Figure S10), thereby demonstrating a certain predominance over the routine liquid electrolyte.…”

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confidence: 99%

Diminishing Space-Charge Layer Effect of Zinc Anodes by an Anion-Immobilized Electrolyte Membrane

Yang

Hua

et al. 2023

ACS Energy Lett.

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The Zn dendrite issue, which is closely related to the creation of the space-charge region upon local anion depletion during cycling, has plagued the practical applications of aqueous Zn metal batteries (ZMBs). Herein, we propose a Kevlar-derived hydrogel (KevlarH) electrolyte with immobilized anions to diminish the space-charge layer effect. SO 4 2− anions are strongly tethered to amide groups of polymer chains, which mitigates the concentration polarization of interfacial Zn 2+ ions by preventing the anion depletion. Furthermore, the relatively weak interaction between Zn 2+ cations and carbonyl groups can redistribute Zn 2+ -ion flux without sacrificing the ion diffusion rate. The synergistic "zincophilic" and "anionphilic" building blocks enable dendrite-free Zn deposition behavior and suppressed side reactions, thereby extending the lifespan of a Zn metal anode up to 3500 h with an ultrahigh Coulombic efficiency of 99.87%. Importantly, the KevlarH electrolyte can be directly used to assemble high-voltage bipolar ZMBs and break the 2 V barrier in aqueous ZMBs.

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confidence: 99%

Diminishing Space-Charge Layer Effect of Zinc Anodes by an Anion-Immobilized Electrolyte Membrane

Yang

Hua

et al. 2023

ACS Energy Lett.

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“…14 A recently published work has explored the use of 2-methyl imidazole, a derivative of imidazole, as the electrolyte additive for alleviating such dendrite issues. 15 It should be noted that realizing cyclable cathodes for ZMBs brings several challenges too, which need to be separately tackled. 16 In this study, our main focus is to study the role of imidazole as an additive in an aqueous 2 M ZnCl 2 solution on active zinc dendrite suppression during electrodeposition, which is one of the major shortcomings of the zinc metal anode in a ZMB.…”

Section: Introductionmentioning

confidence: 99%

“…The most commonly used strategies for the design and optimization of a high-performance zinc metal anode in mildly acidic aqueous electrolytes involve modification of the electrode–electrolyte interface and the use of structural anodes, alloying anodes, intercalation anodes, liquid electrolytes, non-liquid electrolytes, separator design, and other strategies . A recently published work has explored the use of 2-methyl imidazole, a derivative of imidazole, as the electrolyte additive for alleviating such dendrite issues . It should be noted that realizing cyclable cathodes for ZMBs brings several challenges too, which need to be separately tackled …”

Section: Introductionmentioning

confidence: 99%

“…Since the bulky solvation structure has a significant impact on the charge transfer and desolvation kinetics of Zn +2 ions during electrodeposition, it is not favorable for Zn +2 migration and deposition. Thus, it is essential to lessen the degree of solvation, which depends on a number of variables including the anionic salt, the concentration of the electrolyte, and the presence of additives in the electrolyte . The commonly reported anionic salt species currently include SO 4 2– , CF 3 SO 3 – , TFSI – , CH 3 COO – , NO 3 – , Cl – , etc .…”

Section: Introductionmentioning

confidence: 99%

“…Thus, it is essential to lessen the degree of solvation, which depends on a number of variables including the anionic salt, the concentration of the electrolyte, and the presence of additives in the electrolyte. 15 The commonly reported anionic salt species currently include SO 4 2− , CF 3 SO 3 − , TFSI − , CH 3 COO − , NO 3 − , Cl − , etc. 17 It has been shown that CF 3 SO 3 − anions can reduce the number of water molecules in the solvent sheath around Zn +2 , thereby increasing Zn +2 migration, charge transfer kinetics, and the performance of the battery.…”

Section: Introductionmentioning

confidence: 99%

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Mitigating Dendrite Formation on a Zn Electrode in Aqueous Zinc Chloride by the Competitive Surface Chemistry of an Imidazole Additive

Rana

Thakare

Kumar

et al. 2023

ACS Appl. Mater. Interfaces

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Electrochemical energy storage systems are critical in several ways for a smooth transition from nonrenewable to renewable energy sources. Zn-based batteries are one of the promising alternatives to the existing state-of-the-art Li-ion battery technology, since Li-ion batteries pose significant drawbacks in terms of safety and cost-effectiveness. Zn (with a reduction potential of −0.76 V vs SHE) has a significantly higher theoretical volumetric capacity (5851 mAh/cm3) than Li (2061 mAh/cm3), and it is certainly far less expensive, safer, and more earth-abundant. The formation of dendrites, hydrogen evolution, and the formation of a ZnO passivation layer on the Zn anode are the primary challenges in the development and deployment of rechargeable zinc batteries. In this work, we examine the role of imidazole as an electrolyte additive in 2 M ZnCl2 to prevent dendrite formation during zinc electrodeposition via experimental (kinetics and imaging) and theoretical density functional theory (DFT) studies. To characterize the efficacy and to identify the appropriate concentration of imidazole, linear sweep voltammetry (LSV) and chronoamperometry (CA) are performed with in situ monitoring of the electrodeposited zinc. The addition of 0.025 wt % imidazole to 2 M ZnCl2 increases the cycle life of Zn-symmetric cells cycled at 1 mA/cm2 for 60 min of plating and stripping dramatically from 90 to 240 h. A higher value of the nucleation overpotential is noted in the presence of imidazole, which suggests that imidazole is adsorbed at a competitively faster rate on the surface of zinc, thereby suppressing the zinc electrodeposition kinetics and the formation. X-ray tomography reveals that a short circuit caused by dendrite formation is the main plausible failure mechanism of Zn symmetric cells. It is observed that the electrodeposition of zinc is more homogeneous in the presence of imidazole, and its presence in the electrolyte also inhibits the production of a passivating coating (ZnO) on the Zn surface, thereby preventing corrosion. DFT calculations conform well with the stated experimental observations.

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Tailoring Anion Association Strength Through Polycation‐Anion Coordination Mechanism in Imidazole Polymeric Ionic Liquid‐Based Artificial Interphase toward Durable Zn Metal Anodes

Wen

Yang

et al. 2023

Adv Funct Materials

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Artificial interface layer engineering is an efficacious modification strategy for protecting zinc anode from dendrite growth and byproducts formation. However, the high bulk ionic conductivity of most artificial interfacial layers is mainly contributed by the movement of anions (SO 4 2− ), which is the source of parasitic reactions on zinc anode. Herein, a high zinc ion donor transition (σZn 2+ = 3.89 × 10 −2 S cm −1 ) imidazole polymeric ionic liquid interface layer (1-carboxymethyl-3-vinylimidazolium bromide monomer, CVBr) for Zn metal protection is designed. The N + atom of imidazole rings is connected by chains to form the cavities and the anions are confined within these cavities. Thus, the hindering effect of surrounding units on the anions leads to the subdiffusive regime, which inhibits the diffusion of SO 4 2− in interface and increases Zn 2+ transference number. Besides, the polycation-anion co ordination mechanism of PolyCVBr ensures accelerated Zn 2+ transition and realizes rapid internal Zn 2+ migration channel. As a result, the Zn@CVBr||AM symmetry cells deliver high bulk ionic conductivity (4.42 × 10 −2 S cm −1 ) and high Zn 2+ transference number (tZn 2+ = 0.88) simultaneously. The Zn@CVBr||AM-NaV 3 O 8 pouch cells display the capacity retention of 88.9% after 190 cycles under 90° bending, verifying their potential practical application.

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2-methyl imidazole electrolyte additive enabling ultra-stable Zn anode

Cited by 56 publications

References 37 publications

Diminishing Space-Charge Layer Effect of Zinc Anodes by an Anion-Immobilized Electrolyte Membrane

Diminishing Space-Charge Layer Effect of Zinc Anodes by an Anion-Immobilized Electrolyte Membrane

Mitigating Dendrite Formation on a Zn Electrode in Aqueous Zinc Chloride by the Competitive Surface Chemistry of an Imidazole Additive

Tailoring Anion Association Strength Through Polycation‐Anion Coordination Mechanism in Imidazole Polymeric Ionic Liquid‐Based Artificial Interphase toward Durable Zn Metal Anodes

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