Dual-doping for enhancing chemical stability of functional anionic units in sulfide for high-performance all-solid-state lithium batteries

doi:10.1016/j.jechem.2023.07.038

Journal of Energy Chemistry ›› 2023, Vol. 86 ›› Issue (11): 382-390.DOI: 10.1016/j.jechem.2023.07.038

Dual-doping for enhancing chemical stability of functional anionic units in sulfide for high-performance all-solid-state lithium batteries

Peiwen Yu^a, Niaz Ahmad^a,c, Jie Yang^a, Chaoyuan Zeng^c, Xiaoxiao Liang^c, Weiming Huang^e,f,g, Mei Ni^d, Pengcheng Mao^b,*, Wen Yang^a,*

^aKey Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China;
^bAnalysis & Testing Center, Beijing Institute of Technology, Beijing 100081, China;
^cKey Laboratory of Ministry of Education for Advanced Materials in Tropical Island Resources, Hainan Provincial Key Lab of Fine Chemistry, School of Chemical Engineering and Technology, Hainan University, Haikou 570228, Hainan, China;
^dDepartment of Basic Courses, China Fire and Rescue Institute, Beijing 102202, China;
^eCollege of Chemistry, Jilin University, Changchun 130012, Jilin, China;
^fKey Laboratory of Physics and Technology for Advanced Batteries of Ministry of Education, Jilin University, Changchun 130012, Jilin, China;
^gSouthern Marine Science and Engineering Guangdong Lab (Zhanjiang), Zhanjiang 524002, Guangdong, China

Received:2023-06-14 Revised:2023-07-21 Accepted:2023-07-30 Online:2023-11-15 Published:2023-11-07
Contact: *E-mail addresses: pcmao@bit.edu.cn (P. Mao), wenyang@bit.edu.cn (W. Yang).

Abstract

Abstract: The sulfide-based solid-state electrolytes (SEs) reactivity toward moisture and Li-metal are huge barriers that impede their large-scale manufacturing and applications in all-solid-state lithium batteries (ASSLBs). Herein, we proposed an Al and O dual-doped strategy for Li₃PS₄ SE to regulate the chemical/electrochemical stability of anionic PS₄^3- tetrahedra to mitigate structural hydrolysis and parasitic reactions at the SE/Li interface. The optimized Li_3.08Al_0.04P_0.96S_3.92O_0.08 SE presents the highest σ_Li+ of 3.27 mS cm^-1, which is ∼6.8 times higher than the pristine Li₃PS₄ and excellently inhibits the structural hydrolysis for ∼25 min @25% humidity at RT. DFT calculations confirmed that the enhanced chemical stability was revealed to the intrinsically stable entities, e.g., POS₃^3- units. Moreover, Li_3.08Al_0.04P_0.96S_3.92O_0.08 SE cycled stably in Li//Li symmetric cell over 1000 h @0.1 mA cm^-2/0.1 mA h cm^-2, could be revealed to Li-Al alloy and Li₂O at SE/Li interface impeding the growth of Li-dendrites during cycling. Resultantly, LNO@LCO/Li_3.08Al_0.04P_0.96S_3.92O_0.08/Li-In cell delivered initial discharge capacities of 129.8 mA h g^-1 and 83.74% capacity retention over 300 cycles @0.2 C at RT. Moreover, the Li_3.08Al_0.04P_0.96S_3.92O_0.08 SE presented >90% capacity retention over 200 and 300 cycles when the cell was tested with LiNi_0.8Co_0.15Al_0.05O₂ (NCA) cathode material vs. 5 and 10 mg cm^-2 @RT.

Key words: Dual doping, High Li⁺ conductivity, Air-stability, POS₃^3- functional units, Stable SE/electrode interface

Peiwen Yu, Niaz Ahmad, Jie Yang, Chaoyuan Zeng, Xiaoxiao Liang, Weiming Huang, Mei Ni, Pengcheng Mao, Wen Yang. Dual-doping for enhancing chemical stability of functional anionic units in sulfide for high-performance all-solid-state lithium batteries[J]. Journal of Energy Chemistry, 2023, 86(11): 382-390.

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Dual-doping for enhancing chemical stability of functional anionic units in sulfide for high-performance all-solid-state lithium batteries

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