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A salt-concentrated electrolyte for aqueous ammonium-ion hybrid batteries.

ABSTRACT: The development of aqueous ammonium-ion batteries (AAIBs) is currently attracting great attention because of the interesting electrochemical features induced by the charge carrier NH₄⁺. One possible way to improve the performance of AAIBs is increasing the salt concentration in the electrolyte. Yet, few studies focus on the complex electrode-electrolyte interface behaviors in highly concentrated electrolytes, which affect the electrochemical performance of AAIBs significantly. Herein, we aim to understand the impact of CH₃COONH₄ electrolyte concentration on the NH₄⁺ storage performance of a bimetallic hydroxide material. Experimental and theoretical simulation results indicate that the acetate anion will participate in the construction of the solvated NH₄⁺ in a highly concentrated electrolyte, facilitating the adsorption of the solvated NH₄⁺ cluster on the electrode surface. Besides, a new partial de-solvation model is also proposed, demonstrating an energy favorable de-solvation process. Finally, an ammonium-ion hybrid battery is designed, which provides a high average discharge voltage of 1.7 V and good energy density of 368 W h kg_(cathode)^-1, outperforming most of the state-of-the-art aqueous batteries. This work provides new understanding about the electrode's interfacial chemistry in different concentrated CH₃COONH₄ electrolytes, establishes a correlation between the electrolyte concentration and the electrode's performances, and demonstrates the superiority of the hybrid ammonium-ion battery design.

SUBMITTER: Meng J

PROVIDER: S-EPMC10732133 | biostudies-literature | 2023 Dec

REPOSITORIES: biostudies-literature

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A salt-concentrated electrolyte for aqueous ammonium-ion hybrid batteries.

Meng Jianming J Song Yu Y Wang Jing J Hei Peng P Liu Chang C Li Mengxue M Lin Yulai Y Liu Xiao-Xia XX

Chemical science 20231129 1

The development of aqueous ammonium-ion batteries (AAIBs) is currently attracting great attention because of the interesting electrochemical features induced by the charge carrier NH<sub>4</sub><sup>+</sup>. One possible way to improve the performance of AAIBs is increasing the salt concentration in the electrolyte. Yet, few studies focus on the complex electrode-electrolyte interface behaviors in highly concentrated electrolytes, which affect the electrochemical performance of AAIBs significant ...[more]

PMID: 38131066

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Project description:Dual-ion batteries (DIBs) generally operate beyond 4.7 V vs Li+/Li0 and rely on the intercalation of both cations and anions in graphite electrodes. Major challenges facing the development of DIBs are linked to electrolyte decomposition at the cathode-electrolyte interface (CEI), graphite exfoliation, and corrosion of Al current collectors. In this work, X-ray photoelectron spectroscopy (XPS) is employed to gain a broad understanding of the nature and dynamics of the CEI built on anion-intercalated graphite cycled both in highly concentrated electrolytes (HCEs) of common lithium salts (LiPF6, LiFSI, and LiTFSI) in carbonate solvents and in a typical ionic liquid. Though Al metal current collectors were adequately stable in all HCEs, the Coulombic efficiency was substantially higher for HCEs based on LiFSI and LiTFSI salts. Specific capacities ranging from 80 to 100 mAh g-1 were achieved with a Coulombic efficiency above 90% over extended cycling, but cells with LiPF6-based electrolytes were characterized by <70% Coulombic efficiency and specific capacities of merely ca. 60 mAh g-1. The poor performance in LiPF6-containing electrolytes is indicative of the continual buildup of decomposition products at the interface due to oxidation, forming a thick interfacial layer rich in LixPFy, POxFy, LixPOyFz, and organic carbonates as evidenced by XPS. In contrast, insights from XPS analyses suggested that anion intercalation and deintercalation processes in the range from 3 to 5.1 V give rise to scant or extremely thin surface layers on graphite electrodes cycled in LiFSI- and LiTFSI-containing HCEs, even allowing for probing anions intercalated in the near-surface bulk. In addition, ex situ Raman, SEM and TEM characterizations revealed the presence of a thick coating on graphite particles cycled in LiPF6-based electrolytes regardless of salt concentration, while hardly any surface film was observed in the case of concentrated LiFSI and LiTFSI electrolytes.

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A salt-concentrated electrolyte for aqueous ammonium-ion hybrid batteries.

Publications

A salt-concentrated electrolyte for aqueous ammonium-ion hybrid batteries.

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