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| Natura: | Preprint |
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2024
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| Accesso online: | https://arxiv.org/abs/2402.04266 |
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| _version_ | 1866915004865839104 |
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| author | Masese, Titus Kanyolo, Godwill Mbiti Miyazaki, Yoshinobu Tachibana, Shintaro Komori, Sachio Taniyama, Tomoyasu Orikasa, Yuki Saito, Tomohiro |
| author_facet | Masese, Titus Kanyolo, Godwill Mbiti Miyazaki, Yoshinobu Tachibana, Shintaro Komori, Sachio Taniyama, Tomoyasu Orikasa, Yuki Saito, Tomohiro |
| contents | The scarcity of viable electrode and electrolyte materials vastly hinders the advancement of magnesium and calcium batteries. This study utilises solid-state metathetical reactions involving chalcogen- and pnictogen-based honeycomb layered oxides with alkaline-earth halides/nitrates to synthesise $\rm Mg^{2+}$- and $\rm Ca^{2+}$-based materials previously achievable only under high-temperature/high-pressure conditions, as well as new metastable materials with unique crystal versatility. Particularly, we employ metathetical reactions involving $\rm Li_4MgTeO_6$, $\rm Na_2Mg_2TeO_6$, and $\rm Na_4MgTeO_6$ with $\rm MgCl_2$/$\rm MgSO_4$/$\rm Mg(NO_3)_2$.$\rm 6H_2O$ or $\rm Ca(NO_3)_2$.$\rm 4H_2O$ / $\rm CaCl_2$.$\rm 2H_2O$ at temperatures not exceeding 500 $^\circ$C to produce $\rm Mg_3TeO_6$ polymorphs, ilmenite-type $\rm CaMg_2TeO_6$/$\rm Mg_2CaTeO_6$, and double perovskite-type $\rm Ca_2MgTeO_6$. Thus, we demonstrate that these materials, conventionally requiring gigascale pressures or high temperatures (>1000$^\circ$C) for their proper synthesis, are now readily accessible at ambient pressure and considerably lower temperatures. Meanwhile, despite sub-optimal pellet densities, the synthesised ilmenite-type \magenta {$\rm Mg_3TeO_6$ (high-pressure polymorph)} and double perovskite-type ${\rm Ca}_2M{\rm TeO_6}$ ($M = \rm Mg, Ca, Zn$) materials exhibit remarkable bulk ionic conductivity at room temperature, marking them as promising compositional spaces for exploring novel $\rm Mg^{2+}$ and $\rm Ca^{2+}$ conductors. Furthermore, this study extends the applicability of metathetical reactions to attain Mg- or Ca-based antimonates, ruthenates, titanates, phosphates, and silicates, thus opening avenues to novel high-entropy multifunctional nanomaterial platforms with utility in energy storage and beyond. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2402_04266 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Exploring $\rm Mg^{2+}$ and $\rm Ca^{2+}$ Conductors Via Solid-State Metathesis Reactions Masese, Titus Kanyolo, Godwill Mbiti Miyazaki, Yoshinobu Tachibana, Shintaro Komori, Sachio Taniyama, Tomoyasu Orikasa, Yuki Saito, Tomohiro Materials Science The scarcity of viable electrode and electrolyte materials vastly hinders the advancement of magnesium and calcium batteries. This study utilises solid-state metathetical reactions involving chalcogen- and pnictogen-based honeycomb layered oxides with alkaline-earth halides/nitrates to synthesise $\rm Mg^{2+}$- and $\rm Ca^{2+}$-based materials previously achievable only under high-temperature/high-pressure conditions, as well as new metastable materials with unique crystal versatility. Particularly, we employ metathetical reactions involving $\rm Li_4MgTeO_6$, $\rm Na_2Mg_2TeO_6$, and $\rm Na_4MgTeO_6$ with $\rm MgCl_2$/$\rm MgSO_4$/$\rm Mg(NO_3)_2$.$\rm 6H_2O$ or $\rm Ca(NO_3)_2$.$\rm 4H_2O$ / $\rm CaCl_2$.$\rm 2H_2O$ at temperatures not exceeding 500 $^\circ$C to produce $\rm Mg_3TeO_6$ polymorphs, ilmenite-type $\rm CaMg_2TeO_6$/$\rm Mg_2CaTeO_6$, and double perovskite-type $\rm Ca_2MgTeO_6$. Thus, we demonstrate that these materials, conventionally requiring gigascale pressures or high temperatures (>1000$^\circ$C) for their proper synthesis, are now readily accessible at ambient pressure and considerably lower temperatures. Meanwhile, despite sub-optimal pellet densities, the synthesised ilmenite-type \magenta {$\rm Mg_3TeO_6$ (high-pressure polymorph)} and double perovskite-type ${\rm Ca}_2M{\rm TeO_6}$ ($M = \rm Mg, Ca, Zn$) materials exhibit remarkable bulk ionic conductivity at room temperature, marking them as promising compositional spaces for exploring novel $\rm Mg^{2+}$ and $\rm Ca^{2+}$ conductors. Furthermore, this study extends the applicability of metathetical reactions to attain Mg- or Ca-based antimonates, ruthenates, titanates, phosphates, and silicates, thus opening avenues to novel high-entropy multifunctional nanomaterial platforms with utility in energy storage and beyond. |
| title | Exploring $\rm Mg^{2+}$ and $\rm Ca^{2+}$ Conductors Via Solid-State Metathesis Reactions |
| topic | Materials Science |
| url | https://arxiv.org/abs/2402.04266 |