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Enhanced Reversibility of Iron Metal Anode with a Solid Electrolyte Interphase in Concentrated Chloride Electrolytes

Min Soo Jung, Sungjin Yang, Cheng Chen, Sathya Narayanan Jagadeesan, Weiyin Chen, Guangxia Feng, Yiming Sui, Ziang Jiang, Emmanuel N. Musa, Nan‐Chieh Chiu, Hunter Maclennan, Elliot Holden, Kyriakos C. Stylianou, Ju Li, Chong Fang, Xueli Zheng, Xiulei Ji

2025Advanced Materials11 citationsDOIOpen Access PDF

Abstract

Abstract Iron is a promising candidate for a cost‐effective anode for large‐scale energy storage systems due to its natural abundance and well‐established mass production. Recently, Fe‐ion batteries (FeIBs) that use ferrous ions as the charge carrier have emerged as a potential storage solution. The electrolytes in FeIBs are necessarily acidic to render the ferrous ions more anodically stable, allowing a wide operation voltage window. However, the iron anode suffers severe hydrogen evolution reaction with a low Coulombic efficiency (CE) in an acidic environment, shortening the battery cycle life. Herein, a hybrid aqueous electrolyte that forms a solid‐electrolyte interphase (SEI) layer on the Fe anode surface is introduced. The electrolyte mainly comprises FeCl 2 and ZnCl 2 as cosalts, where the Zn‐Cl anionic complex species of the concentrated ZnCl 2 allows dimethyl carbonate (DMC) to be miscible with the aqueous ferrous electrolyte. SEI derived from DMC's decomposition passivates the iron surface, which leads to an average CE of 98.3% and much‐improved cycling stability. This advancement shows the promise of efficient and durable FeIBs.

Topics & Concepts

ElectrolyteAnodeFaraday efficiencyMaterials scienceFerrousInorganic chemistryAqueous solutionElectrochemistryChemical engineeringElectrodeChemistryMetallurgyOrganic chemistryEngineeringPhysical chemistryAdvanced battery technologies researchAdvanced Battery Materials and TechnologiesElectrocatalysts for Energy Conversion