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<p>Efficient lithium extraction is crucial for advancing the global energy transition, yet selective extraction from unconventional resources with high Mg/Li and Na/Li molar ratios remains challenging. Here we report the synthesis of highly oriented [100]-only LiFePO<sub>4</sub> (LFP) nanosheets through an orbital-shielding strategy. This approach employs crown ether molecules to selectively shield specific <i>d</i> orbitals of the central Fe atoms, generating precisely oriented nanosheets with nearly (100) lattice planes. Lithium extraction performance was thoroughly investigated using the representative brines with varying lithium concentrations and interference ion levels from diverse water sources. The Li/Mg and Li/Na selectivity values reach as high as 42,162 and 1,866, with lithium-extraction rates ranging from 1.29 to 7.45 µmol cm<sup>−2</sup> h<sup>−1</sup>. To explore the industrial potential and scalability of the [100]-only LFP nanosheets, an in situ Fe-induced conversion reaction was introduced to replace expensive crown ethers with cost-effective diethylene glycol, enabling kilogram-scale production. A pilot-scale test was conducted using Dead Sea Water brine. The molar Mg/Li and Na/Li were reduced from 800 and 18 to 2.44 × 10<sup>−2</sup> and 3.38 × 10<sup>−2</sup>, respectively, and 44.4 g of battery-grade Li<sub>2</sub>CO<sub>3</sub> was produced during the test. Our orbital-shielding strategy, validated here with LFP, not only provides a potential method for precisely engineering crystal growth such as metal–organic frameworks and Prussian blue analogues but also makes a significantly advanced selective lithium-extraction industry.</p>

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Synthesis of [100]-only LiFePO4 nanosheets for efficient electrochemical lithium extraction from low-grade brines

  • 期刊论文

  • 发表日期：

    2025年12月3日

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  • Shuhao An,
  • Zhen Li,
  • Xin Wang,
  • Ting Xu,
  • Liang Feng,
  • Zhiping Lai

摘要

Efficient lithium extraction is crucial for advancing the global energy transition, yet selective extraction from unconventional resources with high Mg/Li and Na/Li molar ratios remains challenging. Here we report the synthesis of highly oriented [100]-only LiFePO4 (LFP) nanosheets through an orbital-shielding strategy. This approach employs crown ether molecules to selectively shield specific d orbitals of the central Fe atoms, generating precisely oriented nanosheets with nearly (100) lattice planes. Lithium extraction performance was thoroughly investigated using the representative brines with varying lithium concentrations and interference ion levels from diverse water sources. The Li/Mg and Li/Na selectivity values reach as high as 42,162 and 1,866, with lithium-extraction rates ranging from 1.29 to 7.45 µmol cm−2 h−1. To explore the industrial potential and scalability of the [100]-only LFP nanosheets, an in situ Fe-induced conversion reaction was introduced to replace expensive crown ethers with cost-effective diethylene glycol, enabling kilogram-scale production. A pilot-scale test was conducted using Dead Sea Water brine. The molar Mg/Li and Na/Li were reduced from 800 and 18 to 2.44 × 10−2 and 3.38 × 10−2, respectively, and 44.4 g of battery-grade Li2CO3 was produced during the test. Our orbital-shielding strategy, validated here with LFP, not only provides a potential method for precisely engineering crystal growth such as metal–organic frameworks and Prussian blue analogues but also makes a significantly advanced selective lithium-extraction industry.