Structural and compositional characterization of synthetic (Ca,Sr)-tremolite and (Ca,Sr)-diopside solid solutions

Abstract

Tremolite (CaxSr1–x)2Mg5[Si8O22/(OH)2] and diopside (CaxSr1–x)Mg[Si2O6] solid solutions have been synthesized hydrothermally in equilibrium with a 1 molar (Ca,Sr)Cl2 aqueous solution at 750°C and 200 MPa. The solid run products have been investigated by optical, electron scanning and high resolution transmission electron microscopy, electron microprobe, X-ray-powder diffraction and Fourier-transform infrared spectroscopy. The synthesized (Ca,Sr)-tremolites are up to 2000 µm long and 30 µm wide, the (Ca,Sr)-diopsides are up to 150 µm long and 20 µm wide. In most runs the tremolites and diopsides are well ordered and chain multiplicity faults are rare. Nearly pure Sr-tremolite (tr0.02Sr-tr0.98) and Sr-diopside (di0.01Sr-di0.99) have been synthesized. A continuous solid solution series, i.e. complete substitution of Sr2+ for Ca2+ on M4-sites exists for (Ca,Sr)-tremolite. Total substitution of Sr2+ for Ca2+ on M2-sites can be assumed for (Ca,Sr)-diopsides. For (Ca,Sr)-tremolites the lattice parameters a, b and β are linear functions of composition and increase with Sr-content whereas c is constant. For the diopside series all 4 lattice parameters are a linear function of composition; a, b, c increase and β decreases with rising Sr-content. The unit cell volume for tremolite increases 3.47% from 906.68 A3 for tremolite to 938.21 A3 for Sr-tremolite. For diopside the unit cell volume increases 4.87 % from 439.91 A3 for diopside to 461.30 A3 for Sr-diopside. The observed splitting of the OH stretching band in tremolite is caused by different configurations of the next nearest neighbors (multi mode behavior). Resolved single bands can be attributed to the following configurations on the M4-sites: SrSr, SrCa, CaCa and CaMg. The peak positions of these 4 absorption bands are a linear function of composition. They are shifted to lower wavenumbers with increasing Sr-content. No absorption band due to the SrMg configuration on the M4-site is observed. This indicates a very low or negligible cummingtonite component in Sr-rich tremolites, which is also supported by electron microprobe analysis.