Journal Article

PUBDB-2025-02386

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Exploring calcium pillaring of O3-type NaNi$_{0.9}$Ti$_{0.1}$O$_2$ cathodes to advance Na-ion battery technology

An, S.Extern* ; Karger, L.Extern* ; Müller, P.Extern* ; Lin, J.Extern* ; Vasala, S. ; Baran, V.Extern*DESY* ; Dreyer, S. L.Extern* ; Zhang, R.Extern* ; Ulusoy, F.Extern* ; Kondrakov, A. (Corresponding author)Extern* ; Janek, J. (Corresponding author)Extern* ; Brezesinski, T. (Corresponding author)Extern*

2025
Elsevier Amsterdam

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Please use a persistent id in citations: doi:10.1016/j.cej.2025.160939  doi:10.3204/PUBDB-2025-02386

Abstract: NaNi$_{0.9}$Ti$_{0.1}$O$_2$ (NNTO), a promising sodium-ion cathode material, is capable of delivering high specific capacities but is compromised by structural degradation at high potentials and poor redox stability. Herein, we introduced varying amounts of Ca$^{2+}$ as pillaring ions into the intercalation sites of NNTO to examine their effect on structure and electrochemical performance. Laboratory X-ray diffraction and charge/discharge testing identified Na$_{0.95}$Ca$_{0.025}$Ni$_{0.9}$Ti$_{0.1}$O$_2$ (CaNNTO) as the optimal composition in terms of interlayer spacing, rate capability, and cycling stability. Specifically, the capacity retention after 200 cycles improved from 27 to 48 %. To elucidate the role of Ca$^{2+}$, synchrotron X-ray diffraction was performed, revealing that CaNNTO undergoes only about 3 % volume change in the initial cycle, compared to about 30 % for NNTO. This reduced volume variation was confirmed by cross-sectional electron microscopy and acoustic emission measurements. Hard and soft X-ray absorption spectroscopy further indicated a more reversible nickel redox (Ni$^{2+}$/Ni$^{3+}$/Ni$^{4+}$) in CaNNTO, and differential electrochemical mass spectrometry demonstrated that Ca$^{2+}$ incorporation helps suppress oxygen loss from the lattice, thereby directly stabilizing the cathode|electrolyte interface. Overall, calcium pillaring is found to effectively mitigate structural collapse and redox instabilities, making CaNNTO a more viable candidate for practical sodium-ion battery applications.

Note: ISSN 1385-8947 not unique: **2 hits**.

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)
2. Experimentebetreuung PETRA III (FS-PET-D)

Research Program(s):

1. 632 - Materials – Quantum, Complex and Functional Materials (POF4-632) (POF4-632)
2. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
3. FS-Proposal: I-20230867 (I-20230867) (I-20230867)

Experiment(s):

1. PETRA Beamline P02.1 (PETRA III)

Appears in the scientific report 2025

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Database coverage:
; ; ; BIOSIS Previews ; Biological Abstracts ; Clarivate Analytics Master Journal List ; Current Contents - Engineering, Computing and Technology ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 15 ; JCR ; Nationallizenz ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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