Abstract
A synthetic \(\hbox {CaCO}_{3}\)–\(\hbox {SrCO}_{3}\) solid solution with composition \(\hbox {Ca}_{0.82}\hbox {Sr}_{0.18}\) \(\hbox {CO}_{3}\) was investigated by single-crystal X-ray diffraction in the pressure range between 0 and 22 GPa using different pressure-transmitting media. The samples were compressed in DACs using Ne up to \(\sim\)9 GPa and Ar up to \(\sim\)22 GPa. At ambient conditions, \(\hbox {Ca}_{0.82}\hbox {Sr}_{0.18}\) \(\hbox {CO}_{3}\) crystallizes in a monoclinic structure, isostructural to \(\hbox {CaCO}_{3}\)-II, Sr-calcite-II (Sr-CC-II), with space group \(P2_1/c\), 4 formula units per unit cell, Z, \(a = 6.4237(7)\) Å, \(b = 5.0176(1)\) Å, \(c = 8.1129(1)\) Å, \(\beta = 108.064(1)^\circ\) and \(V=248.60(1)\) Å\(^3\) (where the number in parenthesis is 1\(\sigma\) uncertainties on the last digit). At 1.72(5) GPa, a structural phase transition is observed to a new monoclinic structure, Sr-calcite-IIIc (Sr-CC-IIIc), with space group \(P2_1/m\) and \(Z=8\) (\(a~=~6.2683(2)\) Å, \(b = 9.9220(5)\) Å, \(c = 7.6574(6)\) Å, \(\beta = 103.856(6)^\circ\) and \(V = 462.39(5)\) Å\(^3\)), different from any pure \(\hbox {CaCO}_{3}\) polymorph. At 12 GPa, the sample transformed to a triclinic structure, Sr-calcite-IIIb (Sr-CC-IIIb), with space group \(P{\bar{1}}\) and \(Z=4\) ( \(a=6.059(5)\) Å, \(b=6.280(2)\) Å, \(c=6.331(2)\) Å, \(\alpha =95.20(3)^\circ\), \(\beta =108.89(5)^\circ\), \(\gamma =110.52(5)^\circ\) and \(V=207.7(2)\) Å\(^3\)), isostructural to end-member \(\hbox {CaCO}_{3}\)-IIIb. Finally, at 17 GPa, a transition is observed to Sr-calcite-VI (Sr-CC-VI), with space group \(P{\bar{1}}\) and \(Z=2\) (\(a=3.444(3)\) Å, \(b=4.985(4)\) Å, \(c=5.761(5)\) Å, \(\alpha =77.05(7)^\circ\), \(\beta =84.92(7)^\circ\), \(\gamma =89.00(7)^\circ\) and \(V=96.0(1)\) Å\(^3\)), isostructural to end-member \(\hbox {CaCO}_{3}\)-VI, which is preserved up to the maximum investigated pressure of 22 GPa. The results of this study show the effect of Sr/Ca cationic substitution on the high-pressure behavior and physical properties of a \(\hbox {CaCO}_{3}\)–\(\hbox {SrCO}_{3}\) solid solution. The phase evolution of \(\hbox {Ca}_{0.82}\hbox {Sr}_{0.18}\hbox {CO}_3\) and the crystallization of a new phase, Sr-CC-IIIc, different from the high-pressure polymorphs of end-member \(\hbox {CaCO}_{3}\), point to the importance of extending the study of carbonates to more complex systems than pure end-member compositions.
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The data that support the findings of this study are available from the corresponding author, L.P., upon reasonable request.
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Acknowledgements
The research presented in this study has been carried out within the scope of the DFG-funded German research unit DFG FOR 2125 ‘CarboPaT’ (WI1231, SP1216/7-1, BA4020, EF112/1-2, JA1469/11-2, KO1260/16-2). We would like to thank Nico Giordano for assistance in using beamline P02.2 (Petra-III/DESY), Anja Schreiber at GFZ for technical assistance on the FIB and Lkhamsuren Bayarjargal at Goethe University, Frankfurt Am Main, for technical assistance. We are indebted to Bjoern Winkler at Goethe University Frankfurt Am Main, Fabrizio Nestola and Martha Pamato at Universitá degli Studi di Padova for the fruitful discussion.
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Pennacchioni, L., Martirosyan, N.S., Pakhomova, A. et al. Crystal structure and high-pressure phase behavior of a CaCO3–SrCO3 solid solution. Phys Chem Minerals 50, 29 (2023). https://doi.org/10.1007/s00269-023-01252-7
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DOI: https://doi.org/10.1007/s00269-023-01252-7