Fluorine substitution and pre-sodiation strategies to boost energy density of V-based NASICON-structured SIBs: Combined theoretical and experimental study

Lin，Kangshou1; Liu，Qiqi1; Zhou，Yu2; Chen，Hedong4; Liu，Jiefei1; Zhao，Jin Zhu1,3; Hou，Xianhua1,4

2023-05-01

10.1016/j.cej.2023.142464

CHEMICAL ENGINEERING JOURNAL   影响因子和分区

1385-8947

1873-3212

The conventional V-based NASICON-type symmetric sodium-ion batteries (SSIBs) suffer from insufficient energy density mainly due to the low operating voltage. In this study, a novel high-voltage quasi-SSIB (Q-SSIB) was designed by coupling a high-voltage F-substituted cathode (NaV(PO)F@rGO) with a low-voltage pre-sodiated anode (NaV(PO)@rGO) by combining experimental and the first-principles approaches. The electrochemical performance of the cathode was improved by slightly regulating the pH value of the precursor solution to optimize the balance between its crystallization quality and purity, with introducing surface energy analysis to help elucidate the mechanism. An electrochemical pre-intercalation strategy was adopted to synthesize the sodium-rich anode. Besides, the ionic diffusion properties of electrodes were systematically studied by combining DSCV, GITT tests and density functional theory (DFT) calculations, demonstrating that the anode presents faster kinetics in the pre-sodiated phase and shows favorable kinetics compatibility with the cathode. The NaV(PO)//NaV(PO)F Q-SSIB exhibits a high energy density of 340.1 Wh kg and a maximum output voltage plateau of 3.75 V, highly improved compared to the ones (1.8 V, 211 Wh kg) in NaV(PO) SSIBs. This work provides references from theoretical design to experimental study for boosting the energy density of NASICON-type SIBs for broadening their application prospects in energy storage.

High energy density Kinetics Na3V2(PO4)2F3@rGO Na4V2(PO4)3@rGO Sodium-ion battery

SCI ; EI

英语

其他

Joint Fund Project of Guangdong and Guangxi[2020A1515410008] ; National Natural Science Foundation of China[12274145] ; Guangdong Basic and Applied BasicResearch Foundation, China[2023A1515010672]

Engineering

Engineering, Environmental ; Engineering, Chemical

WOS:000967121400001

ELSEVIER SCIENCE SA

20231213778944

Anodes ; Cathodes ; Density functional theory ; Design for testability ; Fluorine ; Metal ions ; Sodium compounds ; Sodium-ion batteries

Metallurgy:531.1 ; Fluid Flow, General:631.1 ; Secondary Batteries:702.1.2 ; Electron Tubes:714.1 ; Chemical Products Generally:804 ; Probability Theory:922.1 ; Classical Physics; Quantum Theory; Relativity:931 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

ENGINEERING

2-s2.0-85150463117

Scopus

1.Guangdong Provincial Key Laboratory of Quantum Engineering and Quantum Materials,Guangdong Engineering Technology Research Center of Efficient Green Energy and Environment Protection Materials,School of Physics and Telecommunication Engineering,South China Normal University,Guangzhou,510006,China
2.School of Energy and Environment,City University of Hong Kong,Hong Kong,999077,Hong Kong
3.Center for Computational Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
4.School of Electronics and Information Engineering,South China Normal University,Foshan,528225,China

Lin，Kangshou,Liu，Qiqi,Zhou，Yu,et al. Fluorine substitution and pre-sodiation strategies to boost energy density of V-based NASICON-structured SIBs: Combined theoretical and experimental study[J]. CHEMICAL ENGINEERING JOURNAL,2023,463.

Lin，Kangshou.,Liu，Qiqi.,Zhou，Yu.,Chen，Hedong.,Liu，Jiefei.,...&Hou，Xianhua.(2023).Fluorine substitution and pre-sodiation strategies to boost energy density of V-based NASICON-structured SIBs: Combined theoretical and experimental study.CHEMICAL ENGINEERING JOURNAL,463.

Lin，Kangshou,et al."Fluorine substitution and pre-sodiation strategies to boost energy density of V-based NASICON-structured SIBs: Combined theoretical and experimental study".CHEMICAL ENGINEERING JOURNAL 463(2023).