Insight into the role of crystallinity in oxide electrolytes enabling high-performance all-solid-state lithium-sulfur batteries

Shiyi Sun; Xiangming Cui; Qianyue Ma; Jianan Wang; Mingbo Ma; Xuhui Yao; Qiong Cai; Jing Li; Xin Chen; Ze Wang; Rui Zhuang; Pengfei Mu; Lei Zhu; Jianwei Liu; Wei Yan

doi:10.1016/j.jcis.2023.07.027

Insight into the role of crystallinity in oxide electrolytes enabling high-performance all-solid-state lithium-sulfur batteries

J Colloid Interface Sci. 2023 Nov 15;650(Pt A):659-668. doi: 10.1016/j.jcis.2023.07.027. Epub 2023 Jul 8.

Authors

Shiyi Sun¹, Xiangming Cui¹, Qianyue Ma², Jianan Wang³, Mingbo Ma⁴, Xuhui Yao⁵, Qiong Cai⁶, Jing Li⁶, Xin Chen¹, Ze Wang¹, Rui Zhuang⁷, Pengfei Mu⁷, Lei Zhu¹, Jianwei Liu¹, Wei Yan⁸

Affiliations

¹ Department of Environmental Science and Engineering, Xi'an Key Laboratory of Solid Waste Recycling and Resource Recovery, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an 710049, PR China.
² Department of Environmental Science and Engineering, Xi'an Key Laboratory of Solid Waste Recycling and Resource Recovery, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an 710049, PR China; Research Institute of Xi'an Jiaotong University, Zhejiang, 328 Wenming Road, Hangzhou 310000, PR China.
³ Department of Environmental Science and Engineering, Xi'an Key Laboratory of Solid Waste Recycling and Resource Recovery, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an 710049, PR China; Research Institute of Xi'an Jiaotong University, Zhejiang, 328 Wenming Road, Hangzhou 310000, PR China; Department of Chemical and Process Engineering, Faculty of Engineering and Physical Sciences, University of Surrey, Guildford GU2 7XH, Surrey, England, United Kingdom. Electronic address: wangjn116@xjtu.edu.cn.
⁴ Xi'an Key Laboratory of Sustainable Energy Materials Chemistry, School of Chemistry, Xi'an Jiaotong University, Xi'an 710049, PR China.
⁵ Advanced Technology Institute, University of Surrey, Guildford, Surrey GU2 7XH, United Kingdom.
⁶ Department of Chemical and Process Engineering, Faculty of Engineering and Physical Sciences, University of Surrey, Guildford GU2 7XH, Surrey, England, United Kingdom.
⁷ Chambroad Chemical Industry Institute Co., Ltd., Boxing Economic Development Zone, 256500 Shandong Province, PR China.
⁸ Department of Environmental Science and Engineering, Xi'an Key Laboratory of Solid Waste Recycling and Resource Recovery, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an 710049, PR China. Electronic address: yanwei@xjtu.edu.cn.

PMID: 37437445
DOI: 10.1016/j.jcis.2023.07.027

Abstract

All-solid-state lithium-sulfur batteries (ASSLSBs) would be a promising candidate for the next-generation batteries due to the utilization of energy-dense electrodes and the non-flammable oxide solid-state electrolytes (SSEs), but still face great challenges such as low ionic conductivity of SSEs, poor interfacial contact and lithium (Li) dendrite propagation. Herein, we regulated the crystallinity degrees of the large-scale-fabricated Li_1.5Al_0.5Ge_1.5(PO₄)₃ (LAGP) SSEs and explored the critical role of crystallinity optimization in reinforcing the basic properties of LAGP, developing a fundamental explanation for the inherent relation between the crystallinity and the performance of ASSLSBs. Benefiting from the optimized crystallinity (∼99.9 %), the large-scale-fabricated LAGP not only realizes the low surface roughness and high ionic conductivity (2.11 × 10^-4 S cm^-1) to improve interfacial contact and reduce resistance in ASSLSBs, but also possesses the dense internal structure with low porosity (1.49 %) to physically resist dendritic propagation and penetration. Consequently, the ASSLSB with the optimized LAGP delivers a high reversible capacity of 647.9 mAh/g even after 150 cycles at 0.1 C. This work confirms the significance of crystallinity in understanding the working mechanisms of oxide SSEs and developing future high-performance ASSLSBs.

Keywords: Crystallinity; Ionic conductivity; Li(1.5)Al(0.5)Ge(1.5)(PO(4))(3); Lithium-sulfur batteries; Solid-state electrolytes.