Highly reversible zinc metal anodes enabled by protonated melamine

Huang, Cong; Zhao, Xin; Hao, Yisu; Yang, Yujie; Yang, Qian; Chang, Ge; Zhang, Yan; Tang, Qunli; Hu, Aiping; Liu, Z.; Chen, Xiaohua

doi:10.1039/d1ta10517e

Cited by 29 publications

(16 citation statements)

References 42 publications

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“…As expected, a larger charge transfer resistance ( R ct ) is recorded after the addition of Cys, indicating the presence of an adsorbed Cys layer, which is consistent with the previous work. [ 5a,9a,21 ] This unique adsorption behavior is believed to be capable of preventing the contact between H 2 O and Zn anodes and thus suppressing the corrosion reaction (Figure 1f).…”

Section: Resultsmentioning

confidence: 99%

Long Shelf‐Life Efficient Electrolytes Based on Trace l‐Cysteine Additives toward Stable Zinc Metal Anodes

Huang

Zhao

Hao

et al. 2022

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The unstable anode/electrolyte interface (AEI) triggers the corrosion reaction and dendrite formation during cycling, hindering the practical application of zinc metal batteries. Herein, for the first time, l‐cysteine (Cys) is employed to serve as an electrolyte additive for stabilizing the Zn/electrolyte interface. It is revealed that Cys additives tend to initially approach the Zn surface and then decompose into multiple effective components for suppressing parasitic reactions and Zn dendrites. As a consequence, Zn|Zn symmetric cells using trace Cys additives (0.83 mm) exhibit a steady cycle life of 1600 h, outperforming that of prior studies. Additionally, an average Coulombic efficiency of 99.6% for 250 cycles is also obtained under critical test conditions (10 mA cm−2/5 mAh cm−2). Cys additives also enable Zn–V2O5 and Zn–MnO2 full cells with an enhanced cycle stability at a low N/P ratio. More importantly, Cys/ZnSO4 electrolytes are demonstrated to be still effective after resting for half year, favoring the practical production.

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Section: Resultsmentioning

confidence: 99%

Long Shelf‐Life Efficient Electrolytes Based on Trace l‐Cysteine Additives toward Stable Zinc Metal Anodes

Huang

Zhao

Hao

et al. 2022

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“…However, the large‐scale application of AZMBs is still hindered by the unstable Zn anode and fast capacity fade, resulting from the uncontrollable dendrite growth and water‐induced side reactions during repeated plating/stripping cycles. [ 5–10 ]…”

Section: Introductionmentioning

confidence: 99%

In Situ Constructing Coordination Compounds Interphase to Stabilize Zn Metal Anode for High‐Performance Aqueous Zn–SeS₂ Batteries

Zhang

et al. 2022

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Aqueous zinc (Zn) metal batteries have been regarded as the most promising aqueous batteries due to their low redox potential, high theoretical capacity, and abundant Zn resources. Unfortunately, Zn dendrite growth and serious side reactions drastically curtail the cycle life, severely affecting their large‐scale application. Herein, a multifunctional ordered Zn‐aminotrimethylene phosphonic acid (Zn‐ATMP) film is in situ modified on the surface of metal Zn via a facile etching process. The modified layer can not only retard the side reactions and suppress the corrosion rate, but also lower the Zn nucleation overpotential and accelerate diffusion and homogenize deposition of Zn2+ due to the strong Zn affinity. Consequently, the as‐prepared Zn‐ATMP@Zn anode in the symmetric cell enables long‐term lifespan (over 1000 h) at 10.0 mA cm−2 with a high areal capacity of 5 mAh cm−2. Furthermore, when assembled with a SeS2‐based cathode, a long lifespan for over 280 cycles at 2 C can be achieved for the aqueous Zn–SeS2 battery. This work provides a reliable strategy for constructing stabilized Zn anode and accelerating the development of an aqueous energy storage system.

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“…As reported before, the current variation at a fixed potential can reflect the diffusion behavior of adsorbed Zn cations or atoms that determine the Zn deposition morphology too. [ 26c,29 ] It is noteworthy that CA curves were collected using the three‐electrode system, where Zn anodes cycled in SA/ZnSO 4 or ZnSO 4 electrolytes were employed as the working electrodes, Pt foils were used as the counter electrodes, and ZnSO 4 solution was adopted as the electrolytes to eliminate the interference of SA additives in the electrolyte. As shown in Figure 5c, for Zn anodes cycled in SA/ZnSO 4 electrolytes, the current increased rapidly and then remained constant, indicating a constrained 2D surface diffusion mechanism, which is favorable to the dendrite‐free Zn deposition.…”

Section: Resultsmentioning

confidence: 99%

Rational Design of Sulfonamide‐Based Additive Enables Stable Solid Electrolyte Interphase for Reversible Zn Metal Anode

Huang

Zhao

et al. 2022

Adv Funct Materials

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The solid electrolyte interphase (SEI)-forming additives strategy is of great significance for improving the cycle stability of zinc (Zn) anodes. Although various additives have been reported, the relationship between their molecular structures and SEI chemistries is poorly understood. Herein, a molecular design principle for sulfonamide-containing additives that endow Zn anodes with a robust SEI layer is proposed. The incorporation of the benzene ring and amino group (−NH 2 ) leads to high adsorption energy, low lowest unoccupied molecular orbital lowest unoccupied molecular orbital (LUMO), and a small highest occupied molecular orbital-LUMO (HOMO-LUMO) gap, facilitating the reduction process of sulfanilamide (SA) additives. Coupled with SA/ZnSO 4 electrolytes, Zn|Zn symmetric cells deliver an ultralong cycle life of 4800 h (200 days) at 2 mA cm −2 and 2 mAh cm −2 . Additionally, a high cumulative plated capacity (CPC) of 6000 mAh cm −2 and 2700 mAh cm −2 is also achieved at a capacity per cycle of 10 mAh cm −2 and 30 mAh cm −2 , respectively. More importantly, the versatility of SA additives is also demonstrated in Zn-V 2 O 5 , Zn-I 2 , and Zn-MnO 2 full cells at a low N/P ratio (the theoretical capacity ratio between the negative and positive electrode) of 5.3, 8.3, and 4.5, respectively. This molecular structure strategy provides a promising path to develop effective SEI-forming additives.

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Highly reversible zinc metal anodes enabled by protonated melamine

Abstract: Zinc anodes have been troubled with serious side reactions and uncontrollable dendrite growth, which is attributed to the unstable electrical double layer (EDL) structure. Herein, a nitrogen−based organic compound named...

Cited by 29 publications

References 42 publications

Long Shelf‐Life Efficient Electrolytes Based on Trace l‐Cysteine Additives toward Stable Zinc Metal Anodes

Long Shelf‐Life Efficient Electrolytes Based on Trace l‐Cysteine Additives toward Stable Zinc Metal Anodes

In Situ Constructing Coordination Compounds Interphase to Stabilize Zn Metal Anode for High‐Performance Aqueous Zn–SeS₂ Batteries

Rational Design of Sulfonamide‐Based Additive Enables Stable Solid Electrolyte Interphase for Reversible Zn Metal Anode

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Highly reversible zinc metal anodes enabled by protonated melamine

Abstract: Zinc anodes have been troubled with serious side reactions and uncontrollable dendrite growth, which is attributed to the unstable electrical double layer (EDL) structure. Herein, a nitrogen−based organic compound named...

Cited by 29 publications

References 42 publications

Long Shelf‐Life Efficient Electrolytes Based on Trace l‐Cysteine Additives toward Stable Zinc Metal Anodes

Long Shelf‐Life Efficient Electrolytes Based on Trace l‐Cysteine Additives toward Stable Zinc Metal Anodes

In Situ Constructing Coordination Compounds Interphase to Stabilize Zn Metal Anode for High‐Performance Aqueous Zn–SeS2 Batteries

Rational Design of Sulfonamide‐Based Additive Enables Stable Solid Electrolyte Interphase for Reversible Zn Metal Anode

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In Situ Constructing Coordination Compounds Interphase to Stabilize Zn Metal Anode for High‐Performance Aqueous Zn–SeS₂ Batteries