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<p>Layered oxides containing redox-capable transition metals find huge application as electrode materials in lithium-ion batteries (LIBs). In the present work, a new series of rock salt superstructured oxides possessing Co<sup>2+</sup>/Co<sup>3+</sup> and Ni<sup>2+</sup>/Ni<sup>3+</sup> redox systems has been explored. The intermediate compositions bridging the Li<sub>3</sub>M<sub>2</sub>SbO<sub>6</sub> and Li<sub>4</sub>MSbO<sub>6</sub> (M = Ni, Co) series have been investigated for their structure, optical and magnetic properties. Le Bail fittings of the PXRD patterns revealed all the compositions Li<sub>3</sub>(Li<sub><i>x</i></sub><InlineEquation ID="IEq1"> <EquationSource Format="TEX">\({\mathbf{M}}_{\bf2-2{\varvec{x}}}^{\bf2+}{\mathbf{M}}_{{\varvec{x}}}^{\bf3+}\)</EquationSource> <EquationSource Format="MATHML"><math> <mrow> <msubsup> <mi mathvariant="bold">M</mi> <mrow> <mn mathvariant="bold">2</mn> <mo>-</mo> <mn mathvariant="bold">2</mn> <mrow> <mi mathvariant="bold">x</mi> </mrow> </mrow> <mrow> <mn mathvariant="bold">2</mn> <mo>+</mo> </mrow> </msubsup> <msubsup> <mi mathvariant="bold">M</mi> <mrow> <mrow> <mi mathvariant="bold-italic">x</mi> </mrow> </mrow> <mrow> <mn mathvariant="bold">3</mn> <mo>+</mo> </mrow> </msubsup> </mrow> </math></EquationSource> </InlineEquation>)SbO<sub>6</sub> (M = Ni, Co and 0.25 ≤ <i>x</i> ≤ 0.75 for Ni and <i>x</i> = 0.75 for Co), have been stabilized in space group <i>C</i>2/<i>m</i>. The systematic evolution of cell volume confirmed uniform introduction of Ni<sup>3+</sup>/Co<sup>3+</sup> ions with increasing Li<sup>+</sup> content. The oxidation states and M<sup>3+</sup>/M<sup>2+</sup> ratios were confirmed from XPS studies and supported by the absorbance bands in UV–visible diffuse reflectance spectra. The temperature-dependent magnetic susceptibility revealed only paramagnetic behaviour with no divergence in ZFC and FC data down to 2 K for both Ni and Co series. The effective magnetic moment decreased systematically with increasing Ni<sup>3+</sup> content. Stabilization of additional compositions, Li<sub>3.75</sub>Ni<sub>0.50</sub>Al<sub>0.75</sub>SbO<sub>6</sub>, Li<sub>3.75</sub>Zn<sub>0.50</sub>Co<sub>0.75</sub>SbO<sub>6</sub> and Li<sub>3.75</sub>Mn<sub>0.50</sub>Fe<sub>0.75</sub>SbO<sub>6</sub> in monoclinic symmetry reinforced the flexibility of the rock salt layered superstructured oxides to produce honeycomb arrays of tailored stoichiometries for diverse applications.</p> Graphical abstract <p></p>

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Evaluation of structural and physical properties of members bridging Li3M2SbO6 and Li4MSbO6 by tuning M2+/M3+ (M = Co, Ni) content

  • 期刊论文

  • 发表日期：

    2026年3月26日

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  • S U Thapliyal,
  • D K Yadav,
  • S Uma

摘要

Layered oxides containing redox-capable transition metals find huge application as electrode materials in lithium-ion batteries (LIBs). In the present work, a new series of rock salt superstructured oxides possessing Co2+/Co3+ and Ni2+/Ni3+ redox systems has been explored. The intermediate compositions bridging the Li3M2SbO6 and Li4MSbO6 (M = Ni, Co) series have been investigated for their structure, optical and magnetic properties. Le Bail fittings of the PXRD patterns revealed all the compositions Li3(Lix \({\mathbf{M}}_{\bf2-2{\varvec{x}}}^{\bf2+}{\mathbf{M}}_{{\varvec{x}}}^{\bf3+}\) M 2 - 2 x 2 + M x 3 + )SbO6 (M = Ni, Co and 0.25 ≤ x ≤ 0.75 for Ni and x = 0.75 for Co), have been stabilized in space group C2/m. The systematic evolution of cell volume confirmed uniform introduction of Ni3+/Co3+ ions with increasing Li+ content. The oxidation states and M3+/M2+ ratios were confirmed from XPS studies and supported by the absorbance bands in UV–visible diffuse reflectance spectra. The temperature-dependent magnetic susceptibility revealed only paramagnetic behaviour with no divergence in ZFC and FC data down to 2 K for both Ni and Co series. The effective magnetic moment decreased systematically with increasing Ni3+ content. Stabilization of additional compositions, Li3.75Ni0.50Al0.75SbO6, Li3.75Zn0.50Co0.75SbO6 and Li3.75Mn0.50Fe0.75SbO6 in monoclinic symmetry reinforced the flexibility of the rock salt layered superstructured oxides to produce honeycomb arrays of tailored stoichiometries for diverse applications.

Graphical abstract