Chloride Insertion Enhances the Electrochemical Oxidation of Iron Hydroxide Double-Layer Hydroxide into Oxyhydroxide in Alkaline Iron Batteries

Jagadeesan, Sathya Narayanan; Barbosa, Gabriel D.; Guo, Fenghua; Zhang, Lihua; Abeykoon, A. M. Milinda; Kwon, Gihan; Olds, Daniel; Turner, Christoffer Heath; Teng, Xiaowei

doi:10.1021/acs.chemmater.3c01496

Title: Chloride Insertion Enhances the Electrochemical Oxidation of Iron Hydroxide Double-Layer Hydroxide into Oxyhydroxide in Alkaline Iron Batteries

Journal Article · Wed Aug 02 00:00:00 EDT 2023 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.3c01496· OSTI ID:2281571

^[1]; Barbosa, Gabriel D. ^[2]; Guo, Fenghua ^[3]; Zhang, Lihua ^[4]; Abeykoon, A. M. Milinda ^[5];

^[5]; Olds, Daniel ^[5];

^[2];

^[1]

Worcester Polytechnic Institute, MA (United States)
Univ. of Alabama, Tuscaloosa, AL (United States)
Univ. of New Hampshire, Durham, NH (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Rechargeable alkaline iron batteries that constitute environmentally benign electrolytes and earth-abundant industrial materials are desirable green solutions for large-scale energy storage. As one of the most abundant metal elements in the earth’s crust, iron (Fe) can satisfy nearly all criteria for low-cost and safe battery electrodes. However, challenges in achieving reversible Fe redox impede their extensive implementation in modern energy supply systems. Here, this study revealed that Cl-anion insertion into Fe(OH)₂ layered double hydroxide (LDH) formed a green rust intermediate phase with the formula [Fe₂²⁺Fe₁³⁺(HO^–)₆]⁺[Cl]^–, which assisted a high Fe(OH)₂/FeOOH conversion reaction (64.7%) and improved cycling stability. This new iron redox chemistry was validated by operando X-ray diffraction, electrochemical testing, X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS) analysis, scanning transmission electron microscopy–energy-dispersive X-ray spectroscopy (STEM-EDS) mapping, and molecular dynamics (MD) simulations. Our study provides new insight into designing LDH materials for high-capacity alkaline iron batteries.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; 2236704

OSTI ID:: 2281571

Report Number(s):: BNL-225185-2024-JAAM

Journal Information:: Chemistry of Materials, Vol. 35, Issue 16; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Chloride Insertion Enhances the Electrochemical Oxidation of Iron Hydroxide Double-Layer Hydroxide into Oxyhydroxide in Alkaline Iron Batteries

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