Synergized Tricomponent All-Inorganics Solid Electrolyte for Highly Stable Solid-State Li-Ion Batteries

Guixiang Xu; Xin Zhang; Shuyang Sun; Yangfan Zhou; Yongfeng Liu; Hangwang Yang; Zhenguo Huang; Fang Fang; Wenping Sun; Zijiang Hong; Mingxia Gao; Hongge Pan

doi:10.1002/advs.202207627

Synergized Tricomponent All-Inorganics Solid Electrolyte for Highly Stable Solid-State Li-Ion Batteries

Adv Sci (Weinh). 2023 Sep;10(25):e2207627. doi: 10.1002/advs.202207627. Epub 2023 Jul 5.

Authors

Guixiang Xu¹, Xin Zhang¹, Shuyang Sun¹, Yangfan Zhou¹, Yongfeng Liu^{1

2}, Hangwang Yang¹, Zhenguo Huang³, Fang Fang⁴, Wenping Sun¹, Zijiang Hong¹, Mingxia Gao¹, Hongge Pan^{1

2}

Affiliations

¹ State Key Laboratory of Silicon and Advanced Semiconductor Materials, Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province and School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310058, China.
² School of Materials Science and Chemical Engineering, Xi'an Technological University, Xi'an, 710021, China.
³ School of Civil & Environmental Engineering, University of Technology Sydney, 81 Broadway, Ultimo, NSW, 2007, Australia.
⁴ Department of Materials Science, Fudan University, Shanghai, 200433, China.

Abstract

Garnet-type oxide Li_6.4 La₃ Zr_1.4 Ta_0.6 O₁₂ (LLZTO) features superior ionic conductivity and good stability toward lithium (Li) metal, but requires high-temperature sintering (≈1200 °C) that induces high fabrication cost, poor mechanical processability, and high interface resistance. Here, a novel high-performance tricomponent composite solid electrolyte (CSE) comprising LLZTO-4LiBH₄ /xLi₃ BN₂ H₈ is reported, which is prepared by ball milling the LLZTO-4LiBH₄ mixture followed by hand milling with Li₃ BN₂ H₈ . Green pellets fabricated by heating the cold-pressed CSE powders at 120 °C offer ultrafast room-temperature ionic conductivity (≈1.73 × 10^-3 S cm^-1 at 30 °C) and ultrahigh Li-ion transference number (≈0.9999), which enable the Li|Li symmetrical cells to cycle over 1600 h at 30 °C with only 30 mV of overpotential. Moreover, the Li|CSE|TiS₂ full cells deliver 201 mAh g^-1 of capacity with long cyclability. These outstanding performances are due to the low open porosity in the electrolyte pellets as well as the high intrinsic ionic conductivity and easy deformability of Li₃ BN₂ H₈ .

Keywords: borohydrides; cyclability; garnet-type oxides; lithium ion batteries; solid-state electrolytes.

Abstract

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