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Inorganic Colloidal Electrolyte for Highly Robust Zinc-Ion Batteries.

ABSTRACT: Zinc-ion batteries (ZIBs) is a promising electrical energy storage candidate due to its eco-friendliness, low cost, and intrinsic safety, but on the cathode the element dissolution and the formation of irreversible products, and on the anode the growth of dendrite as well as irreversible products hinder its practical application. Herein, we propose a new type of the inorganic highly concentrated colloidal electrolytes (HCCE) for ZIBs promoting simultaneous robust protection of both cathode/anode leading to an effective suppression of element dissolution, dendrite, and irreversible products growth. The new HCCE has high Zn²⁺ ion transference number (0.64) endowed by the limitation of SO₄^2-, the competitive ion conductivity (1.1 × 10^-2 S cm^-1) and Zn²⁺ ion diffusion enabled by the uniform pore distribution (3.6 nm) and the limited free water. The Zn/HCCE/α-MnO₂ cells exhibit high durability under both high and low current densities, which is almost 100% capacity retention at 200 mA g^-1 after 400 cycles (290 mAh g^-1) and 89% capacity retention under 500 mA g^-1 after 1000 cycles (212 mAh g^-1). Considering material sustainability and batteries' high performances, the colloidal electrolyte may provide a feasible substitute beyond the liquid and all-solid-state electrolyte of ZIBs.

SUBMITTER: Gao J

PROVIDER: S-EPMC8187543 | biostudies-literature |

REPOSITORIES: biostudies-literature

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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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Inorganic Colloidal Electrolyte for Highly Robust Zinc-Ion Batteries.

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