The role of solid solutions in iron phosphate-based electrodes for selective electrochemical lithium extraction

Gangbin Yan, George Kim, Renliang Yuan, Eli Hoenig, Fengyuan Shi, Wenxiang Chen, Yu Han, Qian Chen, Jian-Min Zuo, Wei Chen and Chong Liu ()
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Gangbin Yan: University of Chicago
George Kim: Illinois Institute of Technology
Renliang Yuan: University of Illinois at Urbana-Champaign
Eli Hoenig: University of Chicago
Fengyuan Shi: University of Illinois Chicago
Wenxiang Chen: University of Illinois at Urbana-Champaign
Yu Han: University of Chicago
Qian Chen: University of Illinois at Urbana-Champaign
Jian-Min Zuo: University of Illinois at Urbana-Champaign
Wei Chen: Illinois Institute of Technology
Chong Liu: University of Chicago

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Electrochemical intercalation can enable lithium extraction from dilute water sources. However, during extraction, co-intercalation of lithium and sodium ions occurs, and the response of host materials to this process is not fully understood. This aspect limits the rational materials designs for improving lithium extraction. Here, to address this knowledge gap, we report one-dimensional (1D) olivine iron phosphate (FePO4) as a model host to investigate the co-intercalation behavior and demonstrate the control of lithium selectivity through intercalation kinetic manipulations. Via computational and experimental investigations, we show that lithium and sodium tend to phase separate in the host. Exploiting this mechanism, we increase the sodium-ion intercalation energy barrier by using partially filled 1D lithium channels via non-equilibrium solid-solution lithium seeding or remnant lithium in the solid-solution phases. The lithium selectivity enhancement after seeding shows a strong correlation with the fractions of solid-solution phases with high lithium content (i.e., LixFePO4 with 0.5 ≤ x

Date: 2022
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DOI: 10.1038/s41467-022-32369-y

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