Approaching theoretical specific capacity of iron-rich lithium iron silicate using graphene-incorporation and fluorine-doping

Liu, Tianwei; Liu, Yadong; Yu, Yikang; Ren, Yang; Sun, Chengjun; Liu, Yuzi; Xu, Jiayi; Liu, Cong; Yang, Zhenzhen; Lu, Wenquan; Ferreira, Paulo; Chao, Zisheng; Xie, Jian

doi:10.1039/d1ta09417c

Title: Approaching theoretical specific capacity of iron-rich lithium iron silicate using graphene-incorporation and fluorine-doping

Journal Article · 16 January 2022 · Journal of Materials Chemistry. A

DOI: https://doi.org/10.1039/d1ta09417c · OSTI ID:1846659

^[1]; Liu, Yadong ^[2];

^[3]; Ren, Yang ^[4]; Sun, Chengjun ^[5]; Liu, Yuzi ^[6]; Xu, Jiayi ^[6];

^[6]; Yang, Zhenzhen ^[6]; Lu, Wenquan ^[6]; Ferreira, Paulo ^[7];

^[8];

^[2]

Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States); Hunan Univ., Changsha (China)
Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States)
Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States); Purdue Univ., West Lafayette, IN (United States)
City Univ. of Hong Kong, Kowloon (Hong Kong)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. of Texas, Austin, TX (United States)
Hunan Univ., Changsha (China)

Lithium iron silicate, Li₂FeSiO₄, is a promising cathode material for lithium ion batteries due to its high theoretical specific capacity, earth abundance, low cost, and environmental friendliness. The challenges of Li₂FeSiO₄ as a practical cathode material are (1) the low electronic and ionic conductivity and (2) the low discharge voltage. The approach of incorporating graphene sheets into the nanostructure of Li₂FeSiO₄ is used for dealing with the low conductivities while fluorine doping is intended to increase the discharge voltage. The fluorine-doped and graphene-incorporated iron-rich lithium iron silicate F-LFSO/G nanomaterials were successfully synthesized using a facile/efficient hydrothermal method with excellent performance, 328.43 mA h g^-1 at 0.1C rate, approaching their theoretical specific capacity, 99% of 331 mA h g^-1. This clearly reveals that the reversible (de)lithiation of 2 Li⁺ ions per F-LFSO has been realized as a result of these approaches. The (de)lithiation process has been studied using in operando high energy synchrotron X-ray absorption near edge spectroscopy and X-ray photoelectron spectroscopy aided by theoretical modeling, which reveals that F doping deeply changes the O electron configuration in F-LFSO, and consequently makes the Li⁺ ion transfer easier, while the reversible redox of oxygen can be utilized to achieve high specific capacity.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1846659

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 8 Vol. 10; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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