Mineral Mimetic Material Sr-Exchanged Sitinakite of Different Crystallinity: Phase Transformations during Heat Treatment and the Strength of SR Fixation in a Ceramic Matrix
Abstract
:1. Introduction
2. Materials and Methods
2.1. Synthesis of Na-Sitinakite
2.2. Synthesis of Sr-Exchanged Forms of Sitinakite
2.3. Mechanism of Sr2+ Incorporation into the Structure of Sitinakite
2.4. Titanate Ceramic Synthesis and Leaching Test
2.5. Material Characterizations
3. Results
3.1. Titanosilicate Characterization
3.2. Ion-Exchange-Induced Transformation
3.3. Phase Transformations of Sr-Exchanged Sitinakite during Heat Treatment
3.4. Leaching Test
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Acknowledgments
Conflicts of Interest
Appendix A
Atom | x | y | z | U(eq) |
---|---|---|---|---|
Ti1 | 3599(2) | 5000 | 1534.0(14) | 12.6(4) |
Ti2 | 5000 | 3613(2) | 3470.0(14) | 14.1(4) |
Si1 | 2500 | 2500 | 2507(3) | 27.5(7) |
Sr2 | 5000 | 1196(4) | 5000 | 18.5(15) |
Sr4 | 1245(10) | 5000 | 0 | 49(3) |
O5 | 6156(9) | 5000 | 3303(7) | 12.5(17) |
O4 | 5000 | 6144(9) | 1710(8) | 21(2) |
O2 | 2459(9) | 3721(6) | 1739(7) | 35.4(18) |
O1 | 3701(6) | 2493(6) | 3289(6) | 20.7(14) |
Sr1 | 5000 | 1401(4) | 1644(5) | 12.9(17) |
O3 | 3539(17) | 5000 | 0 | 44(4) |
O6 | 5000 | 3566(11) | 5000 | 33(4) |
O8 | 6190(30) | 0 | 3387(13) | 120(12) |
O9 | 5000 | 0 | 1733(13) | 155(11) |
Sr3 | 2500 | 2500 | 5000 | 34(3) |
O7 | 2928(17) | 0 | 5000 | 54(4) |
O10 | 1110(20) | 2649(14) | 0 | 155(11) |
Atom | U11 | U22 | U33 | U23 | U13 | U12 |
---|---|---|---|---|---|---|
Ti1 | 21.7(19) | 7.3(15) | 8.8(8) | 0 | −1.8(8) | 0 |
Ti2 | 16(2) | 16.5(17) | 9.9(8) | 1.7(7) | 0 | 0 |
Si1 | 25(3) | 5.6(19) | 51.7(16) | 0 | 0 | −3.9(9) |
Sr2 | 26(3) | 5.1(18) | 24(2) | 0 | 0 | 0 |
Sr4 | 82(8) | 38(5) | 28(4) | 0 | 0 | 0 |
O5 | 14(5) | 10(4) | 13(3) | 0 | 5(3) | 0 |
O4 | 36(7) | 8(4) | 20(3) | 7(3) | 0 | 0 |
O2 | 43(6) | 14(3) | 49(4) | −4(3) | 1(4) | −11(2) |
O1 | 23(4) | 5(3) | 34(3) | 11(2) | −3(3) | 0.6(19) |
Sr1 | 18(4) | 7(3) | 14(3) | −1.7(17) | 0 | 0 |
O3 | 59(14) | 58(12) | 14(5) | 0 | 0 | 0 |
O6 | 78(14) | 15(7) | 5(4) | 0 | 0 | 0 |
O8 | 310(40) | 12(7) | 39(9) | 0 | 35(14) | 0 |
O9 | 410(30) | 45(6) | 15(4) | 0 | 0 | 0 |
Sr3 | 23(4) | 68(7) | 11(3) | 0 | 0 | −4(4) |
O7 | 55(11) | 84(12) | 24(6) | 0 | 0 | 0 |
O10 | 410(30) | 45(6) | 15(4) | 0 | 0 | 0 |
Atom | Atom | Length/Å | Atom | Atom | Length/Å |
---|---|---|---|---|---|
Ti1 | Ti1 1 | 3.076(5) | Sr2 | O6 | 2.602(14) |
Ti1 | Ti2 | 3.1592(17) | Sr2 | O8 8 | 2.666(19) |
Ti1 | Ti2 1 | 3.1592(17) | Sr2 | O8 7 | 2.666(19) |
Ti1 | Sr4 | 3.163(9) | Sr2 | O8 6 | 2.666(19) |
Ti1 | O5 1 | 2.120(8) | Sr2 | O8 | 2.666(19) |
Ti1 | O4 1 | 1.997(6) | Sr2 | O7 | 2.627(16) |
Ti1 | O4 | 1.997(6) | Sr2 | O7 6 | 2.627(16) |
Ti1 | O2 2 | 1.897(7) | Sr4 | Sr4 9 | 2.73(2) |
Ti1 | O2 | 1.897(7) | Sr4 | O2 10 | 2.832(9) |
Ti1 | O3 | 1.8245(17) | Sr4 | O2 11 | 2.832(9) |
Ti2 | Ti2 1 | 3.046(4) | Sr4 | O2 | 2.832(9) |
Ti2 | Sr2 | 3.217(4) | Sr4 | O2 2 | 2.832(9) |
Ti2 | O5 1 | 1.993(6) | Sr4 | Sr1 12 | 2.838(7) |
Ti2 | O5 | 1.993(6) | Sr4 | Sr1 13 | 2.838(7) |
Ti2 | O4 1 | 2.109(10) | Sr4 | O3 | 2.52(2) |
Ti2 | O1 3 | 1.895(6) | Sr4 | O9 12 | 2.472(15) |
Ti2 | O1 | 1.895(6) | Sr4 | O9 13 | 2.472(15) |
Ti2 | Sr1 | 3.256(6) | Sr4 | O10 | 2.586(15) |
Ti2 | O6 | 1.8193(17) | Sr4 | O10 2 | 2.586(15) |
Ti2 | Sr3 4 | 3.5116(11) | O4 | Sr1 1 | 2.696(11) |
Si1 | O2 5 | 1.622(8) | O2 | Sr1 5 | 2.706(10) |
Si1 | O2 | 1.622(8) | O1 | Sr1 | 2.701(9) |
Si1 | O1 | 1.613(6) | O1 | Sr3 | 2.423(7) |
Si1 | O1 5 | 1.613(6) | Sr1 | O8 | 2.89(2) |
Si1 | Sr1 5 | 3.169(3) | Sr1 | O8 8 | 2.89(2) |
Si1 | Sr1 | 3.169(3) | Sr1 | O9 | 1.542(5) |
Si1 | Sr3 | 2.963(4) | Sr1 | O10 14 | 2.527(15) |
Sr2 | Sr2 6 | 2.625(8) | Sr1 | O10 12 | 2.527(15) |
Sr2 | O1 | 2.863(6) | O6 | Sr3 4 | 2.984(5) |
Sr2 | O1 4 | 2.863(6) | O6 | Sr3 | 2.984(5) |
Sr2 | O1 7 | 2.863(6) | Sr3 | O7 15 | 2.784(3) |
Sr2 | O1 3 | 2.863(6) | Sr3 | O7 | 2.784(3) |
Sample | Wt., % ± Δs | |||
---|---|---|---|---|
SiO2 | TiO2 | Fe2O3 | Na2O | |
T-250-Na | 11.0 ± 2.5 | 12.5 ± 2.1 | 1.0 ± 0.5 | 12.4 ± 1.9 |
T-210-Na | 18.4 ± 3.5 | 19.5 ± 3.5 | 2.1 ± 0.9 | 10.8 ± 1.5 |
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Temperature/K | 293 (2) |
---|---|
Crystal system | Orthorhombic |
Spacegroup | Cmmm |
a/Å | 10.9784 (6) |
b/Å | 10.9781 (7) |
c/Å | 11.8861 (7) |
α = β = γ/° | 90 |
Volume/Å3 | 1432.54 (15) |
Z | 4 |
ρcalcg/cm3 | 2.985 |
μ/mm−1 | 6.393 |
F(000) | 1231.0 |
Crystal size/mm3 | 0.14 × 0.14 × 0.14 |
Radiation | MoKα (λ = 0.71073) |
2Θ range for data collection/° | 5.248 to 54.99 |
Index ranges | −14 ≤ h ≤ 14, −14 ≤ k ≤ 14, −14 ≤ l ≤ 15 |
Reflections collected | 8224 |
Independent reflections | 964 [Rint = 0.0414, Rsigma = 0.0139] |
Data/restraints/parameters | 964/0/95 |
Goodness-of-fit on F2 | 1.095 |
Final R indexes [I ≥ 2σ (I)] | R1 = 0.0596, wR2 = 0.1583 |
Final R indexes [all data] | R1 = 0.0631, wR2 = 0.1613 |
Largest diff. peak/hole/e Å−3 | 1.84/−1.27 |
Sample | Wt., % ± Δs | Sorption Capacity, mg/g | H2O Loss | |||||
---|---|---|---|---|---|---|---|---|
SiO2 | TiO2 | Fe2O3 | Na2O | SrO | at 300 °C | at 1000 °C | ||
T-250-Na | 23.1 ± 1.5 | 41.8 ± 1.7 | 2.1 ± 0.9 | 10.6 ± 1.5 | - | - | 11.3 | 13.3 |
T-250-Sr | 24.4 ± 1.9 | 39.7 ± 1.5 | 3.1 ± 1.8 | 3.3 ± 1.1 | 11.7 ± 1.1 | 107.3 | 11.7 | 13.7 |
T-210-Na | 23.7 ± 1.9 | 43.6 ± 2.0 | 3.1 ± 0.9 | 11.4 ± 1.7 | - | - | 13.7 | 15.2 |
T-210-Sr | 22.8 ± 2.1 | 40.2 ± 1.7 | 2.5 ± 0.7 | 2.3 ± 0.9 | 12.2 ± 1.2 | 112.5 | 12.5 | 14.4 |
Sample | Q, mg/g | Leaching Time, day | Desorption in H2O, mg/g | NRi, H2O, g/(m2·day) | Desorption in HNO3, mg/g | NRi, HNO3, g/(m2·day) |
---|---|---|---|---|---|---|
T-250 | 107 | 1 | 6.9 × 10−4 | 4.9 × 10−5 | 13 × 10−2 | 10 × 10−3 |
3 | 11.3 × 10−4 | 2.8 × 10−5 | 31 × 10−2 | 7.9 × 10−3 | ||
T-210 | 112 | 1 | 2.6 × 10−4 | 1.8 × 10−5 | 9 × 10−2 | 6.6 × 10−3 |
3 | 4.2 × 10−4 | 1.0 × 10−5 | 20.7 × 10−2 | 4.9 × 10−3 |
Sample | NRi g/(m2·day) | Conditions: Temperature (°C), Duration (days) | Reference |
---|---|---|---|
Sitinakite-based Sr ceramics | 2.8 × 10−5–1.0 × 10−5 | 25, 3 | Our data |
Perovskite type SrTiO3 | 2 × 10−2–6 × 10−2 | 90, 28 | [57] |
Synroc D | 0.1 × 10−4 | 90, 28 | [58] |
HIP-tailored ceramics | 4 × 10−3 | 90, 28 | [59] |
Synroc MRS | 10−2 | 90, 28 | [60] |
Apatite phosphate ceramics | 10−3–10−4 | 90, 28 | [61] |
Apatite glass-ceramics | 6.9 × 10−4 | 90, 28 | [62] |
Sr0.5Zr2(PO4)3-SmPO4 dual-phase ceramics | 10−4 | 90, 42 | [63] |
Sodium zirconium phosphate | 10−3 | 90, 7 | [64,65] |
Ceramic waste form (SrTiO3) | 29.8 × 10−2 | 90, 7 | [66] |
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Perovskiy, I.A.; Shushkov, D.A.; Ponaryadov, A.V.; Kalashnikova, G.O.; Bazai, A.V.; Bocharov, V.N.; Panikorovskii, T.L. Mineral Mimetic Material Sr-Exchanged Sitinakite of Different Crystallinity: Phase Transformations during Heat Treatment and the Strength of SR Fixation in a Ceramic Matrix. Materials 2024, 17, 1991. https://doi.org/10.3390/ma17091991
Perovskiy IA, Shushkov DA, Ponaryadov AV, Kalashnikova GO, Bazai AV, Bocharov VN, Panikorovskii TL. Mineral Mimetic Material Sr-Exchanged Sitinakite of Different Crystallinity: Phase Transformations during Heat Treatment and the Strength of SR Fixation in a Ceramic Matrix. Materials. 2024; 17(9):1991. https://doi.org/10.3390/ma17091991
Chicago/Turabian StylePerovskiy, Igor A., Dmitry A. Shushkov, Alexey V. Ponaryadov, Galina O. Kalashnikova, Ayya V. Bazai, Vladimir N. Bocharov, and Taras L. Panikorovskii. 2024. "Mineral Mimetic Material Sr-Exchanged Sitinakite of Different Crystallinity: Phase Transformations during Heat Treatment and the Strength of SR Fixation in a Ceramic Matrix" Materials 17, no. 9: 1991. https://doi.org/10.3390/ma17091991