Gulay, Nataliya L, Zanella, Marco 
ORCID: 0000-0002-6164-6169, Robertson, Craig M ORCID: 0000-0002-4789-7607, Ritchie, Daniel, Sonni, Manel ORCID: 0000-0001-6872-445X, Wright, Matthew A, Newnham, Jon A, Hawkins, Cara J, Whitworth, Jayne, Mali, Bhupendra P ORCID: 0000-0002-1699-4877 et al (show 6 more authors)
(2024)
Navigation through high-dimensional chemical space: discovery of Ba5Y13[SiO4]8O8.5 and Ba3Y2[Si2O7]2
CHEMICAL SCIENCE, 15 (40).
pp. 16503-16518.
ISSN 2041-6520, 2041-6539
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Navigation through high-dimensional chemical space discovery of Basub5subYsub13sub[SiOsub4sub]sub8subOsub8.5sub and Basub3su.pdf - Open Access published version Download (3MB) | Preview |
Abstract
Two compounds were discovered in the well-studied BaO–Y<inf>2</inf>O<inf>3</inf>–SiO<inf>2</inf> phase field. Two different experimental routines were used for the exploration of this system due to the differences of synthetic conditions and competition with a glass field. The first phase Ba<inf>5</inf>Y<inf>13</inf>[SiO<inf>4</inf>]<inf>8</inf>O<inf>8.5</inf> was isolated through a combination of energy dispersive X-ray spectroscopy analysis and diffraction techniques which guided the exploration. The second phase Ba<inf>3</inf>Y<inf>2</inf>[Si<inf>2</inf>O<inf>7</inf>]<inf>2</inf> was located using iterative algorithmic identification of target compositions. The structure solution of the new compounds was aided by continuous rotation electron diffraction, and the structures were refined against combined synchrotron and neutron time-of-flight powder diffraction. Ba<inf>5</inf>Y<inf>13</inf>[SiO<inf>4</inf>]<inf>8</inf>O<inf>8.5</inf> crystallizes in I4̄2m, a = 18.92732(1), c = 5.357307(6) Å and represents its own structure type which combines elements of structures of known silicates embedded in columns of interconnected yttrium-centred polyhedra characteristic of high-pressure phases. Ba<inf>3</inf>Y<inf>2</inf>[Si<inf>2</inf>O<inf>7</inf>]<inf>2</inf> has P2<inf>1</inf> symmetry with a pseudo-tetragonal cell (a = 16.47640(4), b = 9.04150(5), c = 9.04114(7) Å, b = 90.0122(9)°) and is a direct superstructure of the Ca<inf>3</inf>BaBi[P<inf>2</inf>O<inf>7</inf>]<inf>2</inf> structure. Despite the lower symmetry, the structure of Ba<inf>3</inf>Y<inf>2</inf>[Si<inf>2</inf>O<inf>7</inf>]<inf>2</inf> retains disorder in both Ba/Y sites and disilicate network, thus presenting a superposition of possible locally-ordered fragments. Ba<inf>5</inf>Y<inf>13</inf>[SiO<inf>4</inf>]<inf>8</inf>O<inf>8.5</inf> has low thermal conductivity of 1.04(5) W m−1 K−1 at room temperature. The two discovered phases provide a rich structural platform for further functional material design. The interplay of automated unknown phase composition identification with multiple diffraction methods offers acceleration of the time-consuming exploration of high-dimensional chemical spaces for new structures.
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | 3402 Inorganic Chemistry, 34 Chemical Sciences |
| Divisions: | Faculty of Science & Engineering Faculty of Science & Engineering > School of Physical Sciences |
| Depositing User: | Symplectic Admin |
| Date Deposited: | 07 Nov 2024 14:25 |
| Last Modified: | 16 Jun 2026 17:07 |
| DOI: | 10.1039/d4sc04440a |
| Related Websites: | |
| URI: | https://livrepository.liverpool.ac.uk/id/eprint/3187111 |
| Disclaimer: | The University of Liverpool is not responsible for content contained on other websites from links within repository metadata. Please contact us if you notice anything that appears incorrect or inappropriate. |
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