Reaction Mechanism of Na-Ion Deintercalation in Na$_{\textrm{2}}$CoSiO$_{\textrm{4}}$. Wang, J., Hoteling, G., Shepard, R., Wahila, M., Wang, F., Smeu, M., & Liu, H. The Journal of Physical Chemistry C, 126(40):16983 – 16992, October, 2022.
doi  abstract   bibtex   
Sodium transition metal silicates are potential candidate electrode materials to enable two-electron redox per transition metal ion center. Yet, the electrochemical reaction mechanism remains elusive despite the widely reported electrochemical activity for this class of materials as intercalation cathodes for Na-ion batteries. Adopting monoclinic Na$_{\textrm{2}}$CoSiO$_{\textrm{4}}$ as a model compound, we used high-resolution synchrotron X-ray diffraction (XRD) and X-ray pair distribution function (PDF) analysis to elucidate the structure of the partially de-sodiated Na$_{\textrm{2-x}}$CoSiO$_{\textrm{4}}$ phases for the Co$^{\textrm{3+}}$/Co$^{\textrm{2+}}$ redox couple. The appearance of satellite reflections in the intermediate Na$_{\textrm{1.5}}$CoSiO$_{\textrm{4}}$ and NaCoSiO$_{\textrm{4}}$ phases manifests the formation of modulated structures, which are induced by Na$^{\textrm{+}}$/vacancy and Co$^{\textrm{2+}}$/Co$^{\textrm{3+}}$ charge orderings. Accounting for these structural orderings is important to understand the function and performance of sodium transition metal silicate electrodes.
@article{wang_reaction_2022,
	title = {Reaction {Mechanism} of {Na}-{Ion} {Deintercalation} in {Na}$_{\textrm{2}}${CoSiO}$_{\textrm{4}}$},
	volume = {126},
	copyright = {All rights reserved},
	issn = {1932-7447},
	doi = {10.1021/acs.jpcc.2c05314},
	abstract = {Sodium transition metal silicates are potential candidate electrode materials to enable two-electron redox per transition metal ion center. Yet, the electrochemical reaction mechanism remains elusive despite the widely reported electrochemical activity for this class of materials as intercalation cathodes for Na-ion batteries. Adopting monoclinic Na$_{\textrm{2}}$CoSiO$_{\textrm{4}}$ as a model compound, we used high-resolution synchrotron X-ray diffraction (XRD) and X-ray pair distribution function (PDF) analysis to elucidate the structure of the partially de-sodiated Na$_{\textrm{2-x}}$CoSiO$_{\textrm{4}}$ phases for the Co$^{\textrm{3+}}$/Co$^{\textrm{2+}}$ redox couple. The appearance of satellite reflections in the intermediate Na$_{\textrm{1.5}}$CoSiO$_{\textrm{4}}$ and NaCoSiO$_{\textrm{4}}$ phases manifests the formation of modulated structures, which are induced by Na$^{\textrm{+}}$/vacancy and Co$^{\textrm{2+}}$/Co$^{\textrm{3+}}$ charge orderings. Accounting for these structural orderings is important to understand the function and performance of sodium transition metal silicate electrodes.},
	number = {40},
	journal = {The Journal of Physical Chemistry C},
	author = {Wang, Jiwei and Hoteling, Grayson and Shepard, Robert and Wahila, Matthew and Wang, Fei and Smeu, Manuel and Liu, Hao},
	month = oct,
	year = {2022},
	pages = {16983 -- 16992},
}

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