Atomistic insights into the screening and role of oxygen in enhancing the Li+ conductivity of Li7P3S11-: XOx solid-state electrolytes

Liu，Hanghui1,2; Yang，Zhenhua1,2; Wang，Qun1,2; Wang，Xianyou3; Shi，Xingqiang4

2019

10.1039/c9cp05329h

PHYSICAL CHEMISTRY CHEMICAL PHYSICS   影响因子和分区

1463-9076

1463-9084

Herein, we implement first-principles calculations to design LiPSO at an atomic scale, aiming to obtain stable LiPSO-type solid electrolyte materials with good Li conductivity. After searching for chemical potentials, LiO is expected to be the potential raw material, and it can afford the most favorable growth environment for the synthesis of LiPSO (x = 0.25, 0.50, 0.75 and 1). Among these compounds, it is found that LiPSO exhibits the most desirable Li conductivity of 109 mS cm at 300 K, which is far higher than that of LiPS (50 mS cm at 300 K). By structural analysis, it is demonstrated that the Li diffusion pathway in LiPSO is significantly broadened relative to that in LiPS (71.38 Åvs. 69.48 Å), which breaks the bottleneck during Li diffusion. Moreover, the resistance of Li ion diffusion in LiPSO decreases due to the balance of interactions between Li and its neighbouring atoms at the transition state, which induces a much lesser energy barrier of LiPSO than that of LiPS (0.20 eV vs. 0.31 eV). Moreover, introducing Li vacancies is unlikely to alter the essence of the inherent superionic conductivity of LiPSO. Furthermore, LiPSO can maintain good thermal stability and similar electrochemical stability to LiPS. This study successfully clarifies the role of oxygen in enhancing the Li conductivity of LiPSO. Moreover, it affords a new strategy to design other solid-state electrolytes with good Li conductivity.

SCI ; EI

英语

其他

Shenzhen Fundamental Research Foundation[JCY20170817105007999]

Chemistry ; Physics

Chemistry, Physical ; Physics, Atomic, Molecular & Chemical

WOS:000502767400006

ROYAL SOC CHEMISTRY

20201708553218

Sulfur compounds ; Calculations ; Solid electrolytes ; Lithium ; Lithium compounds ; Diffusion

Lithium and Alloys:542.4 ; Alkali Metals:549.1 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Mathematics:921

CHEMISTRY

2-s2.0-85076381849

Scopus

1.Key Laboratory of Materials Design and Preparation Technology of Hunan Province,School of Materials Science and Engineering,Xiangtan University,Xiangtan, Hunan,411105,China
2.Key Laboratory of Low Dimensional Materials and Application Technology (Ministry of Education),School of Materials Science and Engineering,Xiangtan University,Xiangtan, Hunan,411105,China
3.National Local Joint Engineering Laboratory for Key Materials of New Energy Storage Battery,National Base for International Science and Technology Cooperation,Hunan Province Key Laboratory of Electrochemical Energy Storage and Conversion,School of Chemistry,Xiangtan University,Xiangtan, Hunan,411105,China
4.Department of Physics,Southern University of Science and Technology,Shenzhen,518055,China

Liu，Hanghui,Yang，Zhenhua,Wang，Qun,et al. Atomistic insights into the screening and role of oxygen in enhancing the Li+ conductivity of Li7P3S11-: XOx solid-state electrolytes[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2019,21(48):26358-26367.

Liu，Hanghui,Yang，Zhenhua,Wang，Qun,Wang，Xianyou,&Shi，Xingqiang.(2019).Atomistic insights into the screening and role of oxygen in enhancing the Li+ conductivity of Li7P3S11-: XOx solid-state electrolytes.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,21(48),26358-26367.

Liu，Hanghui,et al."Atomistic insights into the screening and role of oxygen in enhancing the Li+ conductivity of Li7P3S11-: XOx solid-state electrolytes".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 21.48(2019):26358-26367.