Recrystallization and Uptake of 226Ra into Ba-Rich (Ba,Sr)SO4 Solid Solutions
Abstract
:1. Introduction
2. Materials and Methods
3. Results
3.1. The Evolution of the 226Ra Concentration over Time
3.2. The Evolution of Ba and Sr Concentrations over Time
3.3. Chemical and Microstructural Evolution of the Solid
- (1)
- XSrSO4 = 5 mol%, 23 °C, S/L = 0.5 g/kg, slow macroscopic recrystallization kinetics;
- (2)
- XSrSO4 = 29 mol%, 23 °C, S/L = 0.5 g/kg, fast macroscopic recrystallization kinetics and 226Ra entrapment;
- (3)
- XSrSO4 = 5 mol%, 90 °C, 5 g/kg, fast macroscopic recrystallization kinetics, no entrapment of 226Ra.
4. Discussion
4.1. Effect of XSrSO4 upon the Solubility of 226Ra
4.2. Kinetics of the Recrystallization from (Ba,Sr)SO4 to (Ba,Sr,Ra)SO4
5. Conclusions
Author Contributions
Funding
Acknowledgments
Conflicts of Interest
Appendix A
Day | Ra Concentration in Solution (10−8 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_0.5 g/kg_RT | (Ba0.83Sr0.17)SO4_0.5 g/kg_RT | (Ba0.71Sr0.29)SO4_0.5 g/kg_RT | |
0.5 | 536 | 523 | 559 |
1 | 542 | 442 | 355 |
3 | 551 | 433 | 324 |
7 | 550 | 406 | 280 |
14 | 568 | 431 | 268 |
21 | 569 | 404 | 223 |
30 | 580 | 357 | 148 |
42 | 571 | 302 | 2.30 |
56 | 600 | 247 | 0.18 |
70 | 625 | 79.4 | 0.14 |
98 | 556 | 0.61 | 0.35 |
133 | 605 | 0.47 | 0.35 |
161 | 544 | 0.51 | 0.37 |
224 | 568 | 0.63 | 0.41 |
294 | 438 | 0.34 | 0.41 |
406 | 264 | 0.65 | 0.49 |
525 | 12.5 | 0.68 | 0.51 |
664 | 20.9 | 0.72 | 0.61 |
Equilibrium (GEMS) | 3.24 | 1.13 | 0.76 |
Day | Ra Concentration (10−8 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_0.5 g/kg_70 | (Ba0.83Sr0.17)SO4_0.5 g/kg_70 | (Ba0.71Sr0.29)SO4_0.5 g/kg_70 | |
0.5 | 546 | 534 | 531 |
1 | 552 | 441 | 222 |
3 | 539 | 402 | 80.0 |
7 | 559 | 281 | 0.45 |
14 | 576 | 1.66 | |
21 | 519 | 0.61 | |
30 | 378 | 0.45 | |
42 | 58.3 | 0.47 | 0.37 |
56 | 23.1 | 0.45 | |
70 | 21.5 | 0.47 | |
98 | 20.9 | 0.29 | 0.61 |
133 | 21.3 | 0.72 | 1.06 |
161 | 21.7 | 0.76 | 1.51 |
224 | 22.5 | 0.85 | 2.25 |
294 | 19.2 | 1.46 | 3.27 |
406 | 26.4 | 4.30 | 4.70 |
525 | 24.7 | 6.95 | 5.32 |
664 | 23.5 | 0.11 | 7.16 |
Equilibrium (GEMS) | 16.2 | 6.55 | 4.59 |
Day | Ra Concentration (10−8 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_0.5 g/kg_90 | (Ba0.83Sr0.17)SO4_0.5 g/kg_90 | (Ba0.71Sr0.29)SO4_0.5 g/kg_90 | |
0.5 | 546 | 541 | 532 |
1 | 547 | 308 | 30.5 |
3 | 576 | 72.2 | 0.41 |
7 | 522 | ||
14 | 344 | 0.55 | |
21 | 80.8 | ||
30 | 36.2 | ||
42 | 19.8 | 0.22 | 0.45 |
56 | 17.0 | ||
70 | 17.6 | ||
98 | 14.1 | 0.41 | 0.51 |
133 | 14.0 | 0.38 | |
161 | 15.7 | 0.36 | 2.64 |
224 | 15.8 | 0.67 | 3.35 |
294 | 16.1 | 1.70 | 3.11 |
406 | 24.2 | 3.35 | 6.95 |
525 | 25.6 | 3.35 | 7.43 |
664 | 31.6 | 4.31 | 9.10 |
Equilibrium (GEMS) | 24.9 | 10.6 | 7.78 |
Day | Ra Concentration (10−8 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_5 g/kg_90 | (Ba0.83Sr0.17)SO4_5 g/kg_90 | (Ba0.71Sr0.29)SO4_5 g/kg_90 | |
0.5 | 507 | 503 | 490 |
1 | 55.4 | 1.02 | 0.86 |
42 | 0.43 | 0.41 | 0.37 |
98 | 0.41 | 0.45 | 0.51 |
406 | 0.43 | 0.43 | 0.51 |
664 | 1.10 | 0.79 | 0.89 |
Equilibrium (GEMS) | 0.62 | 0.49 | 0.57 |
Day | Ba Concentration (10−6 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_0.5 g/kg_RT | (Ba0.83Sr0.17)SO4_0.5 g/kg_RT | (Ba0.71Sr0.29)SO4_0.5 g/kg_RT | |
1 | 20.9 | 12.9 | |
3 | 27.4 | 15.7 | 19.1 |
7 | 26.6 | 13.1 | 9.83 |
14 | 26.5 | 12.2 | 9.00 |
21 | 27.6 | 12.5 | 8.21 |
30 | 27.1 | 11.4 | 7.45 |
42 | 30.0 | 10.9 | 7.41 |
56 | 31.9 | 11.0 | 6.06 |
70 | 31.1 | 11.1 | 4.62 |
98 | 32.3 | 8.40 | 3.27 |
133 | 32.3 | 5.91 | 3.35 |
161 | 33.1 | 5.69 | 3.53 |
224 | 32.2 | 4.51 | 2.79 |
294 | 32.2 | 3.81 | 2.52 |
406 | 31.9 | 3.69 | 2.32 |
525 | 20.2 | 2.79 | 1.92 |
664 | 20.9 | 3.26 | 2.35 |
Equilibrium (GEMS) | 9.40 | 2.90 | 1.70 |
Day | Ba Concentration (10−6 mol/kg) | ||
---|---|---|---|
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_RT | Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_RT | Reference (Ba0.71Sr0.29)SO4_0.5 g/kg_RT | |
1 | 22.7 | 7.06 | 6.39 |
3 | 26.3 | 6.70 | 6.11 |
7 | 23.3 | 6.41 | 5.10 |
14 | 1.82 | 5.83 | 4.59 |
21 | 23.1 | 5.90 | 0.08 |
30 | 29.9 | 5.17 | 0.17 |
42 | 23.6 | 4.95 | 3.75 |
56 | 22.7 | 4.81 | 3.88 |
70 | 26.2 | 4.95 | 3.60 |
98 | 24.2 | 4.00 | 2.77 |
133 | 22.6 | 4.08 | 4.35 |
161 | 24.0 | 3.86 | 3.02 |
224 | 22.4 | 3.50 | 2.53 |
294 | 25.0 | 3.13 | 2.41 |
406 | 25.0 | 3.27 | 2.18 |
525 | 22.4 | 2.77 | 1.74 |
664 | 24.4 | 2.92 | 1.94 |
Equilibrium (GEMS) | 9.05 | 2.87 | 1.69 |
Day | Ba Concentration (10−6 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_0.5 g/kg_70 | (Ba0.83Sr0.17)SO4_0.5 g/kg_70 | (Ba0.71Sr0.29)SO4_0.5 g/kg_70 | |
1 | 50.0 | 22.7 | 21.3 |
3 | 49.3 | 26.7 | 14.5 |
7 | 13.9 | 9.69 | |
14 | 50.0 | 16.4 | 7.88 |
21 | 47.2 | 12.7 | 6.53 |
30 | 52.0 | 9.63 | 6.11 |
42 | 42.5 | 8.37 | 5.64 |
56 | 48.8 | 9.74 | 5.85 |
70 | 37.3 | 9.45 | 5.68 |
98 | 37.3 | 7.19 | 5.28 |
133 | 56.3 | 5.67 | 7.41 |
161 | 37.5 | 7.81 | 5.40 |
224 | 27.3 | 6.90 | 5.10 |
294 | 35.5 | 4.66 | |
406 | 36.1 | 6.83 | 5.19 |
525 | 29.3 | 5.26 | 4.26 |
664 | 31.7 | 6.08 | 4.98 |
Equilibrium (GEMS) | 26.6 | 9.42 | 5.62 |
Day | Ba Concentration (10−6 mol/kg) | ||
---|---|---|---|
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_70 | Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_70 | Reference (Ba0.71Sr0.29)SO4_0.5 g/kg_70 | |
1 | 38.0 | 14.3 | 13.2 |
3 | 52.7 | 15.6 | 7.88 |
7 | 34.0 | 13.7 | 5.42 |
14 | 34.1 | 14.6 | 5.91 |
21 | 33.5 | 12.6 | 5.57 |
30 | 31.7 | 11.8 | 5.04 |
42 | 32.1 | 11.3 | 2.41 |
56 | 30.4 | 10.5 | 4.66 |
70 | 32.8 | 10.6 | 5.32 |
98 | 32.0 | 9.54 | 4.56 |
133 | 33.1 | 9.32 | 5.08 |
161 | 31.8 | 8.81 | 5.24 |
224 | 31.3 | 7.72 | 4.91 |
294 | 32.0 | 6.63 | 0.85 |
406 | 33.1 | 5.96 | 4.66 |
525 | 29.1 | 5.03 | 4.07 |
664 | 30.8 | 5.85 | 4.52 |
Equilibrium (GEMS) | 2.58 | 9.29 | 5.58 |
Day | Ba Concentration (10−6 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_0.5 g/kg_90 | (Ba0.83Sr0.17)SO4_0.5 g/kg_90 | (Ba0.71Sr0.29)SO4_0.5 g/kg_90 | |
1 | 56.2 | 90.3 | 17.2 |
3 | 51.8 | 25.8 | 10.7 |
7 | 52.5 | 16.8 | 8.60 |
14 | 51.2 | 12.6 | 7.86 |
21 | 46.4 | 9.17 | 6.07 |
30 | 44.6 | 10.4 | 6.74 |
42 | 40.7 | 7.73 | 5.50 |
56 | 38.9 | 8.52 | 5.80 |
70 | 43.0 | 9.40 | 6.69 |
98 | 42.2 | 8.69 | 6.15 |
133 | 43.1 | 8.74 | 6.29 |
161 | 43.3 | 8.96 | 6.79 |
224 | 42.9 | 8.72 | 6.66 |
294 | 36.8 | 6.73 | 4.70 |
406 | 41.8 | 7.98 | 6.40 |
525 | 40.4 | 7.96 | 5.73 |
664 | 42.6 | 8.72 | 6.29 |
Equilibrium (GEMS) | 32.9 | 12.2 | 7.39 |
Day | Ba Concentration (10−6 mol/kg) | ||
---|---|---|---|
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_90 | Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_90 | Reference (Ba0.71Sr0.29)SO4_0.5 g/kg_90 | |
1 | 43.5 | 15.6 | 8.69 |
3 | 43.3 | 12.1 | 6.74 |
7 | 44.1 | 11.0 | 5.94 |
14 | 45.2 | 10.4 | 5.87 |
21 | 42.0 | 7.99 | 4.23 |
30 | 43.1 | 8.69 | 5.07 |
42 | 41.8 | 7.09 | 4.20 |
56 | 42.2 | 7.72 | |
70 | 42.0 | 8.61 | 5.34 |
98 | 42.2 | 8.26 | 5.04 |
133 | 43.4 | 8.39 | 4.98 |
161 | 44.1 | 9.20 | 5.57 |
224 | 46.3 | 9.11 | 5.29 |
294 | 43.9 | 7.32 | 4.51 |
406 | 42.1 | 8.49 | 5.20 |
525 | 40.5 | 8.76 | 11.6 |
664 | 38.2 | 9.30 | 13.2 |
Equilibrium (GEMS) | 32.0 | 12.1 | 0.32 |
Day | Ba concentration (10−6 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_5 g/kg_90 | (Ba0.83Sr0.17)SO4_5 g/kg_90 | (Ba0.71Sr0.29)SO4_5 g/kg_90 | |
1 | 30.9 | 7.81 | 7.59 |
3 | 27.2 | 8.33 | 8.32 |
7 | 20.7 | 7.14 | 6.45 |
14 | 18.6 | 6.81 | 6.28 |
21 | 13.8 | 5.04 | 4.70 |
30 | 15.8 | 5.93 | 5.46 |
42 | 12.1 | 5.72 | 4.67 |
56 | 9.66 | 5.12 | 3.60 |
70 | 13.6 | 6.11 | 5.77 |
98 | 12.5 | 0.00 | 4.82 |
133 | 12.6 | 4.95 | 5.15 |
161 | 12.6 | 5.59 | 5.72 |
224 | 11.6 | 5.19 | 4.75 |
294 | 7.72 | 3.60 | 3.63 |
406 | 8.15 | 3.56 | 3.33 |
525 | 7.64 | 3.51 | 3.35 |
664 | 8.97 | 3.99 | 3.60 |
Equilibrium (GEMS) | 7.37 | 4.16 | 4.16 |
Day | Ba concentration (10−6 mol/kg) | ||
---|---|---|---|
Reference (Ba0.95Sr0.05)SO4_5 g/kg_90 | Reference (Ba0.83Sr0.17)SO4_5 g/kg_90 | Reference (Ba0.71Sr0.29)SO4_5 g/kg_90 | |
1 | 25.2 | 5.46 | 5.25 |
3 | 16.7 | 6.30 | 5.80 |
7 | 14.0 | 5.26 | 5.09 |
14 | 14.2 | 5.18 | 5.10 |
21 | 11.1 | 3.86 | 4.09 |
30 | 12.9 | 4.34 | 4.85 |
42 | 10.2 | 4.17 | 3.97 |
56 | 9.22 | 3.60 | 3.63 |
70 | 11.6 | 4.81 | 4.70 |
98 | 11.9 | 4.46 | 4.38 |
133 | 11.7 | 4.46 | 4.63 |
161 | 13.8 | 4.96 | 5.00 |
224 | 12.3 | 4.52 | 4.43 |
294 | 10.9 | 3.80 | 3.41 |
406 | 11.2 | 3.91 | 4.09 |
525 | 11.6 | 4.46 | 4.31 |
664 | 13.2 | 6.05 | 5.57 |
Equilibrium (GEMS) | 6.97 | 4.19 | 4.19 |
Day | Sr Concentration (10−5 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_0.5 g/kg_RT | (Ba0.83Sr0.17)SO4_0.5 g/kg_RT | (Ba0.71Sr0.29)SO4_0.5 g/kg_RT | |
1 | 0.92 | 15.7 | 17.5 |
3 | 0.81 | 12.2 | 29.7 |
7 | 0.85 | 10.6 | 17.3 |
14 | 0.79 | 10.3 | 18.9 |
21 | 0.77 | 10.9 | 17.9 |
30 | 0.82 | 11.2 | 18.3 |
42 | 0.78 | 11.2 | 19.6 |
56 | 0.90 | 11.1 | 23.7 |
70 | 0.87 | 11.1 | 28.9 |
98 | 0.84 | 13.9 | 33.2 |
133 | 0.84 | 18.1 | 37.7 |
161 | 0.90 | 19.8 | 40.2 |
224 | 0.85 | 22.3 | 42.3 |
294 | 0.86 | 25.3 | 44.2 |
406 | 1.13 | 26.6 | 44.0 |
525 | 2.51 | 26.6 | 45.1 |
664 | 3.16 | 28.2 | 49.3 |
Equilibrium (GEMS) | 10.8 | 37.4 | 65.2 |
Day | Sr Concentration (10−5 mol/kg) | ||
---|---|---|---|
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_RT | Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_RT | Reference (Ba0.71Sr0.29)SO4_0.5 g/kg_RT | |
1 | 0.95 | 10.7 | 21.4 |
3 | 0.98 | 10.1 | 22.0 |
7 | 0.12 | 10.8 | 22.1 |
14 | 0.67 | 40.6 | 21.9 |
21 | 0.88 | 12.7 | 15.9 |
30 | 13.4 | 14.6 | |
42 | 1.17 | 13.9 | 33.6 |
56 | 0.77 | 14.4 | 32.4 |
70 | 0.90 | 15.3 | 34.2 |
98 | 4.20 | 16.6 | 35.0 |
133 | 0.51 | 18.9 | 56.1 |
161 | 0.74 | 17.9 | 39.9 |
224 | 0.85 | 19.3 | 42.3 |
294 | 0.75 | 20.2 | 43.5 |
406 | 1.08 | 24.4 | 43.7 |
525 | 0.90 | 21.9 | 42.7 |
664 | 0.88 | 24.2 | 44.6 |
Equilibrium (GEMS) | 10.8 | 37.5 | 65.4 |
Day | Sr Concentration (10−5 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_0.5 g/kg_70 | (Ba0.83Sr0.17)SO4_0.5 g/kg_70 | (Ba0.71Sr0.29)SO4_0.5 g/kg_70 | |
1 | 1.00 | 11.6 | 23.7 |
3 | 1.10 | 14.45 | 23.1 |
7 | 2.32 | 12.1 | 30.7 |
14 | 1.05 | 15.0 | 44.3 |
21 | 1.09 | 21.6 | 47.1 |
30 | 1.45 | 25.8 | 50.5 |
42 | 2.52 | 27.3 | 52.7 |
56 | 3.73 | 33.2 | 54.3 |
70 | 3.42 | 36.6 | 51.9 |
98 | 3.65 | 34.4 | 55.1 |
133 | 6.22 | 36.3 | 68.0 |
161 | 4.13 | 36.8 | 55.2 |
224 | 4.61 | 39.5 | 57.6 |
294 | 4.49 | 39.7 | 55.8 |
406 | 4.75 | 74.0 | 50.4 |
525 | 5.32 | 42.8 | 48.5 |
664 | 6.21 | 36.2 | 50.9 |
Equilibrium (GEMS) | 10.7 | 37.0 | 64.0 |
Day | Sr Concentration (10−5 mol/kg) | ||
---|---|---|---|
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_70 | Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_70 | Reference (Ba0.71Sr0.29)SO4_0.5 g/kg_70 | |
1 | 1.59 | 11.8 | 39.4 |
3 | 2.27 | 13.5 | 34.1 |
7 | 1.70 | 14.5 | 38.0 |
14 | 1.50 | 16.9 | 42.0 |
21 | 1.72 | 16.0 | 47.1 |
30 | 1.78 | 16.3 | 48.4 |
42 | 2.66 | 16.7 | 49.6 |
56 | 2.04 | 17.6 | 51.4 |
70 | 2.20 | 18.4 | 54.1 |
98 | 2.27 | 20.0 | 52.4 |
133 | 2.36 | 21.7 | 59.7 |
161 | 2.35 | 22.9 | 56.1 |
224 | 2.53 | 22.1 | 54.8 |
294 | 2.41 | 26.6 | 19.8 |
406 | 2.75 | 31.4 | 48.7 |
525 | 1.63 | 28.9 | 46.0 |
664 | 1.77 | 28.3 | 56.6 |
Equilibrium (GEMS) | 10.7 | 37.1 | 64.4 |
Day | Sr Concentration (10−5 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_0.5 g/kg_90 | (Ba0.83Sr0.17)SO4_0.5 g/kg_90 | (Ba0.71Sr0.29)SO4_0.5 g/kg_90 | |
1 | 0.69 | 43.2 | 22.6 |
3 | 0.99 | 13.5 | 28.0 |
7 | 1.20 | 16.2 | 35.7 |
14 | 1.35 | 21.0 | 39.8 |
21 | 2.00 | 24.1 | 42.5 |
30 | 2.57 | 26.4 | 43.6 |
42 | 2.95 | 28.2 | |
56 | 3.19 | 29.6 | 52.5 |
70 | 3.35 | 31.1 | 49.9 |
98 | 3.32 | 31.2 | 47.9 |
133 | 3.53 | 31.4 | 47.4 |
161 | 3.57 | 31.1 | 43.3 |
224 | 3.72 | 32.9 | 47.5 |
294 | 3.74 | 32.9 | 47.2 |
406 | 3.98 | 37.0 | 56.1 |
525 | 4.60 | 33.7 | 48.7 |
664 | 5.40 | 37.9 | 65.3 |
Equilibrium (GEMS) | 10.7 | 36.7 | 62.7 |
Day | Sr Concentration (10−5 mol/kg) | ||
---|---|---|---|
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_90 | Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_90 | Reference (Ba0.71Sr0.29)SO4_0.5 g/kg_90 | |
1 | 1.40 | 11.9 | 26.0 |
3 | 1.27 | 13.9 | 37.6 |
7 | 1.34 | 16.8 | 35.2 |
14 | 1.35 | 18.9 | 38.7 |
21 | 1.43 | 20.4 | 41.7 |
30 | 1.25 | 21.0 | 41.8 |
42 | 1.45 | 22.1 | 43.4 |
56 | 1.48 | 23.4 | |
70 | 1.40 | 24.5 | 47.4 |
98 | 1.60 | 13.3 | 48.6 |
133 | 1.54 | 26.0 | 46.1 |
161 | 1.75 | 25.6 | 45.6 |
224 | 1.66 | 26.8 | 48.4 |
294 | 1.91 | 27.0 | 48.7 |
406 | 1.90 | 31.1 | 50.6 |
525 | 1.63 | 28.9 | 46.0 |
664 | 1.77 | 28.3 | 56.6 |
Equilibrium (GEMS) | 10.7 | 36.7 | 63.3 |
Day | Sr Concentration (10−5 mol/kg) | ||
---|---|---|---|
(Ba0.95Sr0.05)SO4_5 g/kg_90 | (Ba0.83Sr0.17)SO4_5 g/kg_90 | (Ba0.71Sr0.29)SO4_5 g/kg_90 | |
1 | 8.81 | 37.3 | 42.1 |
3 | 10.6 | 45.0 | 51.7 |
7 | 12.7 | 48.2 | 55.2 |
14 | 16.0 | 51.0 | 60.7 |
21 | 17.5 | 52.6 | 59.9 |
30 | 18.5 | 54.9 | 61.5 |
42 | 20.3 | 64.6 | 61.5 |
56 | 21.3 | 77.7 | 64.1 |
70 | 21.9 | 56.9 | 68.3 |
98 | 22.2 | 66.6 | |
133 | 23.0 | 58.1 | 68.0 |
161 | 23.3 | 59.0 | 72.4 |
224 | 23.7 | 60.5 | 71.4 |
294 | 23.3 | 60.1 | 68.2 |
406 | 28.4 | 74.9 | 85.0 |
525 | 35.7 | 74.7 | 77.3 |
664 | 36.2 | 70.9 | 77.4 |
Equilibrium (GEMS) | 63.1 | 113 | 113 |
Day | Sr Concentration (10−5 mol/kg) | ||
---|---|---|---|
Reference (Ba0.95Sr0.05)SO4_5 g/kg_90 | Reference (Ba0.83Sr0.17)SO4_5 g/kg_90 | Reference (Ba0.71Sr0.29)SO4_5 g/kg_90 | |
1 | 9.60 | 38.9 | 40.1 |
3 | 11.3 | 40.6 | 46.3 |
7 | 12.8 | 47.1 | 50.8 |
14 | 14.0 | 44.9 | 52.0 |
21 | 14.7 | 51.2 | 55.3 |
30 | 16.1 | 53.5 | 58.2 |
42 | 16.1 | 55.0 | 55.7 |
56 | 16.6 | 50.9 | 57.5 |
70 | 17.5 | 55.1 | 59.2 |
98 | 42.7 | 57.0 | 59.3 |
133 | 18.0 | 60.4 | 60.1 |
161 | 17.9 | 56.8 | 60.0 |
224 | 18.3 | 58.7 | 60.0 |
294 | 18.4 | 50.7 | 60.8 |
406 | 20.8 | 66.1 | 71.7 |
525 | 18.7 | 65.9 | 85.9 |
664 | 18.2 | 61.3 | 71.1 |
Equilibrium (GEMS) | 66.8 | 114 | 114 |
Day | Particle | XSrSO4 | XRaSO4 | XBaSO4 |
---|---|---|---|---|
(%) | (%) | (%) | ||
(Ba0.95Sr0.05)SO4_0.5 g/kg_RT | ||||
1 | P1 | 4.6 | <0.5 | 95.1 |
P2 | 4.5 | 0.8 | 94.7 | |
P3 | 4.8 | <0.5 | 95.0 | |
P4 | 3.5 | 0.6 | 95.9 | |
P5 | 9.8 | n.d. | 90.2 | |
Average EDX | 5.4 | 94.2 | ||
Average mass balance | 5.6 | 0.04 | 95.4 | |
42 | P1 | 7.3 | <0.5 | 92.5 |
P1 | 3.9 | <0.5 | 95.8 | |
P2 | 3.9 | <0.5 | 95.9 | |
P3 | 3.5 | 0.5 | 96.0 | |
P3 | 8.2 | 0.5 | 91.3 | |
P4 | 6.0 | <0.5 | 93.8 | |
P5 | 2.9 | <0.5 | 96.9 | |
Average EDX | 5.1 | 94.6 | ||
Average mass balance | 4.7 | 0.03 | 95.3 | |
98 | P1 | 3.7 | n.d. | 96.3 |
P1 | 3.2 | n.d. | 96.8 | |
P2 | 10.1 | <0.5 | 89.8 | |
P2 | 10.3 | <0.5 | 89.4 | |
P3 | 5.0 | n.d. | 95.0 | |
P4 | 3.3 | <0.5 | 96.5 | |
P5 | 4.7 | <0.5 | 95.0 | |
Average EDX | 5.8 | 94.1 | ||
Average mass balance | 4.7 | 0.03 | 95.3 | |
664 | P1 | 4.1 | <0.5 | 95.7 |
P1 | 4.2 | <0.5 | 95.7 | |
P2 | 3.6 | <0.5 | 96.2 | |
P2 | 4.4 | <0.5 | 95.2 | |
P3 | 5.7 | <0.5 | 93.9 | |
P3 | 7.0 | <0.5 | 92.8 | |
P4 | 3.8 | <0.5 | 95.9 | |
P4 | 4.1 | <0.5 | 95.6 | |
P5 | 5.0 | <0.5 | 94.7 | |
P5 | 4.5 | 0.7 | 94.9 | |
P5 | 2.8 | 1.2 | 95.8 | |
P6 | 5.5 | <0.5 | 93.8 | |
P6 | 5.8 | <0.5 | 93.9 | |
P7 | 3.4 | <0.5 | 96.4 | |
P7 | 4.1 | <0.5 | 95.7 | |
P7 | 2.0 | 0.5 | 97.5 | |
P8 | 0.4 | 0.7 | 98.9 | |
P8 | 1.3 | 1.2 | 97.5 | |
P8 | 1.2 | 2.7 | 95.3 | |
P9 | 1.3 | 0.8 | 97.9 | |
P9 | 6.6 | 0.7 | 93.4 | |
Average EDX | 3.8 | 95.6 | ||
Average mass balance | 3.6 | 0.03 | 96.1 | |
Calculated equilibrium | 0.3 | 0.02 | 99.7 |
Day | Particle | XSrSO4 | XRaSO4 | XBaSO4 |
---|---|---|---|---|
(%) | (%) | (%) | ||
(Ba0.71Sr0.29)SO4_0.5 g/kg_RT | ||||
1 | P1 | 27.4 | n.d. | 72.6 |
P1 | 5.8 | <0.5 | 93.8 | |
P1 | 20.8 | <0.5 | 78.9 | |
P2 | 9.2 | <0.5 | 90.7 | |
P2 | 8.1 | 0.5 | 91.5 | |
P3 | 30.5 | <0.5 | 69.3 | |
P3 | 27.4 | n.d. | 72.6 | |
P3 | 22.3 | <0.5 | 77.4 | |
P4 | 9.0 | <0.5 | 90.5 | |
P4 | 15.8 | 1.59 | 82.6 | |
P5 | 23.9 | <0.5 | 75.8 | |
P6 | 4.3 | <0.5 | 95.4 | |
Average EDX | 17.0 | 82.6 | ||
Average mass balance | 23.2 | 0.1 | 76.6 | |
42 | P1 | 6.5 | 1.1 | 92.8 |
P1 | 21.6 | <0.5 | 78.0 | |
P2 | 8.4 | <0.5 | 91.1 | |
P3 | 7.3 | 2.8 | 89.9 | |
P3 | 5.4 | 2.4 | 92.2 | |
P4 | 11.2 | 1.1 | 87.8 | |
P4 | 27.9 | <0.5 | 71.7 | |
P5 | 23.1 | <0.5 | 76.7 | |
P5 | 9.1 | 0.6 | 90.3 | |
Average EDX | 13.4 | 85.6 | ||
Average mass balance | 22.3 | 0.3 | 77.4 | |
98 | P1 | 7.9 | 0.9 | 91.2 |
P2 | 22.7 | <0.5 | 76.9 | |
P2 | 17.6 | <0.5 | 82.2 | |
P2 | 6.9 | <0.5 | 92.8 | |
P3 | 11.8 | <0.5 | 87.8 | |
P3 | 15.4 | <0.5 | 84.5 | |
P4 | 17.3 | 0.7 | 82.0 | |
P5 | 12.9 | 1.0 | 86.1 | |
P6 | 11.9 | 0.9 | 87.3 | |
P6 | 24.3 | <0.5 | 75.3 | |
P6 | 14.8 | <0.5 | 84.8 | |
Average EDX | 14.1 | 85.4 | ||
Average mass balance | 16.9 | 0.3 | 82.8 | |
664 | P1 | 9.9 | 0.6 | 89.6 |
P1 | 9.8 | 0.5 | 89.7 | |
P2 | 11.6 | 0.5 | 87.9 | |
P2 | 10.5 | <0.5 | 89.3 | |
P3 | 7.8 | <0.5 | 91.9 | |
P4 | 7.2 | <0.5 | 92.5 | |
P4 | 8.1 | 0.5 | 91.4 | |
P4 | 8.9 | n.d. | 91.1 | |
P5 | 21.4 | <0.5 | 78.4 | |
P5 | 5.0 | <0.5 | 94.6 | |
P5 | 9.0 | <0.5 | 90.9 | |
P5 | 11.7 | 0.7 | 87.6 | |
P6 | 9.0 | <0.5 | 90.7 | |
P6 | 5.2 | <0.5 | 94.5 | |
P6 | 8.4 | <0.5 | 91.3 | |
P7 | 5.3 | 0.5 | 94.2 | |
P7 | 10.3 | <0.5 | 89.4 | |
P7 | 4.7 | <0.5 | 95.0 | |
P8 | 8.2 | <0.5 | 91.5 | |
P8 | 10.0 | 1.4 | 88.6 | |
P8 | 7.4 | <0.5 | 92.2 | |
P9 | 21.3 | <0.5 | 78.3 | |
P9 | 10.0 | 0.5 | 89.5 | |
P10 | 9.6 | 0.8 | 89.6 | |
P10 | 17.4 | <0.5 | 82.3 | |
Average EDX | 9.9 | 89.7 | ||
Average mass balance | 9.5 | 0.4 | 90.2 | |
Calculated equilibrium | 0.6 | 0.3 | 99.1 |
Day | Particle | XSrSO4 | XRaSO4 | XBaSO4 |
---|---|---|---|---|
(%) | (%) | (%) | ||
(Ba0.95Sr0.05)SO4_5 g/kg_90 | ||||
1 | P1 | 10.3 | <0.5 | 89.5 |
P1 | 12.8 | n.d | 87.2 | |
P1 | 13.6 | <0.5 | 86.5 | |
P2 | 10.1 | n.d | 89.9 | |
P2 | 3.9 | 1.7 | 94.4 | |
P3 | 4.0 | <0.5 | 95.6 | |
P4 | 4.9 | <0.5 | 94.6 | |
Average EDX | 8.5 | 91.1 | ||
Average mass balance | 4.6 | 0.03 | 95.4 | |
42 | P1 | 4.1 | 0.5 | 95.4 |
P1 | 1.5 | 0.7 | 97.1 | |
P2 | 2.0 | <0.5 | 97.8 | |
P3 | 4.0 | <0.5 | 95.9 | |
P4 | 1.0 | <0.5 | 98.8 | |
Average EDX | 2.5 | 97.0 | ||
Average mass balance | 4.1 | 0.03 | 95.9 | |
98 | P1 | 2.6 | <0.5 | 97.2 |
P2 | 1.6 | 0.98 | 97.4 | |
P3 | 1.5 | <0.5 | 98.2 | |
P4 | 7.0 | <0.5 | 91.8 | |
P5 | 0.8 | <0.5 | 99.0 | |
P6 | 4.4 | <0.5 | 95.5 | |
Average EDX | 3.0 | 96.5 | ||
Average mass balance | 4.0 | 0.03 | 96.0 | |
664 | P1 | 3.4 | <0.5 | 96.3 |
P2 | 6.3 | n.d | 93.7 | |
P2 | 6.0 | <0.5 | 93.8 | |
P3 | 3.1 | <0.5 | 96.5 | |
P3 | 2.3 | 0.6 | 97.1 | |
P4 | 4.4 | <0.5 | 95.2 | |
P4 | 5.0 | <0.5 | 94.9 | |
P5 | 1.6 | <0.5 | 98.0 | |
P5 | 2.7 | <0.5 | 97.2 | |
P6 | 5.8 | <0.5 | 94.0 | |
P6 | 3.8 | <0.5 | 95.9 | |
P7 | 2.2 | 0.5 | 97.3 | |
P8 | 4.8 | <0.5 | 95.0 | |
P9 | 3.2 | 0.6 | 96.2 | |
Average EDX | 3.9 | 95.8 | ||
Average mass balance | 3.4 | 0.03 | 96.6 | |
Calculated equilibrium | 2.2 | 0.02 | 97.8 |
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Solid Solution | XBaSO4 | XSrSO4 |
---|---|---|
(Ba0.95Sr0.05)SO4 | 0.95 | 0.05 ± 20% |
(Ba0.83Sr0.17)SO4 | 0.83 | 0.17 ± 20% |
(Ba0.71Sr0.29)SO4 | 0.71 | 0.29 ± 20% |
Name | Solid/Liquid | c(Ra) | Temperature |
---|---|---|---|
(g/kg) | (10−6 mol/kg) | (°C) | |
(Ba0.95Sr0.05)SO4_0.5 g/kg_RT | 0.5 | 5 | 23 ± 2 |
(Ba0.83Sr0.17)SO4_0.5 g/kg_RT | 0.5 | 5 | 23 ± 2 |
(Ba0.71Sr0.29)SO4_0.5 g/kg_RT | 0.5 | 5 | 23 ± 2 |
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_RT | 0.5 | 0 | 23 ± 2 |
Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_RT | 0.5 | 0 | 23 ± 2 |
Reference (Ba0.71Sr0.29)SO4_0.5 g/kg_RT | 0.5 | 0 | 23 ± 2 |
(Ba0.95Sr0.05)SO4_0.5 g/kg_70 | 0.5 | 5 | 70 |
(Ba0.83Sr0.17)SO4_0.5 g/kg_70 | 0.5 | 5 | 70 |
(Ba0.71Sr0.29)SO4_0.5 g/kg_70 | 0.5 | 5 | 70 |
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_70 | 0.5 | 0 | 70 |
Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_70 | 0.5 | 0 | 70 |
Reference (Ba0.71Sr0.29)SO4_0.5 g/L_70 | 0.5 | 0 | 70 |
(Ba0.95Sr0.05)SO4_0.5 g/kg_90 | 0.5 | 5 | 90 |
(Ba0.83Sr0.17)SO4_0.5 g/kg_90 | 0.5 | 5 | 90 |
(Ba0.71Sr0.29)SO4_0.5 g/kg_90 | 0.5 | 5 | 90 |
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_90 | 0.5 | 0 | 90 |
Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_90 | 0.5 | 0 | 90 |
Reference (Ba0.71Sr0.29)SO4_0.5 g/kg_90 | 0.5 | 0 | 90 |
(Ba0.95Sr0.05)SO4_5 g/kg_90 | 5.0 | 5 | 90 |
(Ba0.83Sr0.17)SO4_5 g/kg_90 | 5.0 | 5 | 90 |
(Ba0.71Sr0.29)SO4_5 g/kg_90 | 5.0 | 5 | 90 |
Reference (Ba0.95Sr0.05)SO4_5 g/kg_90 | 5.0 | 0 | 90 |
Reference (Ba0.83Sr0.17)SO4_5 g/kg_90 | 5.0 | 0 | 90 |
Reference (Ba0.71Sr0.29)SO4_5 g/kg_90 | 5.0 | 0 | 90 |
Experiment | Composition of Solid Solution Present at Equilibrium | ||
---|---|---|---|
XBaSO4 | XRaSO4 (%) | XSrSO4 | |
(Ba0.95Sr0.05)SO4_0.5 g/kg_RT | 99.74 | 0.24 | 0.02 |
(Ba0.83Sr0.17)SO4_0.5 g/kg_RT | 99.52 | 0.27 | 0.21 |
(Ba0.71Sr0.29)SO4_0.5 g/kg_RT | 99.06 | 0.31 | 0.63 |
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_RT | 99.99 | - | 0.01 |
Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_RT | 99.83 | - | 0.17 |
Reference (Ba0.71Sr0.29)SO4_0.5 g/kg_RT | 99.49 | - | 0.51 |
(Ba0.95Sr0.05)SO4_0.5 g/kg_70 | 99.72 | 0.24 | 0.04 |
(Ba0.83Sr0.17)SO4_0.5 g/kg_70 | 99.29 | 0.27 | 0.44 |
(Ba0.71Sr0.29)SO4_0.5 g/kg_70 | 98.34 | 0.30 | 1.36 |
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_70 | 99.96 | - | 0.04 |
Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_70 | 99.63 | - | 0.37 |
Reference (Ba0.71Sr0.29)SO4_0.5 g/L_70 | 98.88 | - | 1.12 |
(Ba0.95Sr0.05)SO4_0.5 g/kg_90 | 99.69 | 0.23 | 0.07 |
(Ba0.83Sr0.17)SO4_0.5 g/kg_90 | 99.17 | 0.26 | 0.57 |
(Ba0.71Sr0.29)SO4_0.5 g/kg_90 | 97.60 | 0.30 | 2.10 |
Reference (Ba0.95Sr0.05)SO4_0.5 g/kg_90 | 99.94 | - | 0.06 |
Reference (Ba0.83Sr0.17)SO4_0.5 g/kg_90 | 99.42 | - | 0.58 |
Reference (Ba0.71Sr0.29)SO4_0.5 g/kg_90 | 98.24 | - | 1.76 |
(Ba0.95Sr0.05)SO4_5 g/kg_90 | 97.83 | 0.02 | 2.15 |
(Ba0.83Sr0.17)SO4_5 g/kg_90 | 90.21 | 0.02 | 9.77 |
(Ba0.71Sr0.29)SO4_5 g/kg_90 | 90.20 | 0.03 | 9.77 |
Reference (Ba0.95Sr0.05)SO4_5 g/kg_90 | 98.02 | - | 1.98 |
Reference (Ba0.83Sr0.17)SO4_5 g/kg_90 | 92.55 | - | 7.45 |
Reference (Ba0.71Sr0.29)SO4_5 g/kg_90 | 92.55 | - | 7.45 |
Day | Method | Number of Particles EDS-Analyses | XSrSO4 Minimum | XSrSO4 Maximum | XSrSO4 Average | |
---|---|---|---|---|---|---|
(%) | (%) | (%) | ||||
(Ba0.95Sr0.05)SO4_0.5 g/kg_RT | ||||||
1 | EDX | 5 | 5 | 3.5 | 9.8 | 6.2 |
Mass balance | 4.6 | |||||
42 | EDX | 5 | 7 | 2.9 | 8.2 | 5.0 |
Mass balance | 4.7 | |||||
98 | EDX | 5 | 7 | 3.2 | 10.3 | 5.8 |
Mass balance | 4.7 | |||||
664 | EDX | 9 | 21 | 0.4 | 9.8 | 4.1 |
Mass balance | 3.6 | |||||
Calculated equilibrium | 0.3 | |||||
(Ba0.71Sr0.29)SO4_0.5 g/kg_RT | ||||||
1 | EDX | 6 | 12 | 4.3 | 30.5 | 17.0 |
Mass balance | 23.2 | |||||
42 | EDX | 5 | 9 | 5.4 | 27.9 | 13.4 |
Mass balance | 22.3 | |||||
98 | EDX | 6 | 11 | 6.9 | 24.3 | 14.1 |
Mass balance | 16.9 | |||||
664 | EDX | 10 | 25 | 4.7 | 21.4 | 9.9 |
Mass balance | 9.5 | |||||
Calculated equilibrium | 0.6 | |||||
(Ba0.95Sr0.05)SO4_5 g/kg_90 | ||||||
1 | EDX | 4 | 7 | 3.9 | 13.6 | 8.5 |
Mass balance | 4.6 | |||||
42 | EDX | 4 | 5 | 1 | 4.1 | 2.5 |
Mass balance | 4.1 | |||||
98 | EDX | 6 | 6 | 0.8 | 7 | 3.0 |
Mass balance | 4.0 | |||||
664 | EDX | 9 | 14 | 1.6 | 6.3 | 3.9 |
Mass balance | 3.4 | |||||
Calculated equilibrium | 2.2 |
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Brandt, F.; Klinkenberg, M.; Poonoosamy, J.; Bosbach, D. Recrystallization and Uptake of 226Ra into Ba-Rich (Ba,Sr)SO4 Solid Solutions. Minerals 2020, 10, 812. https://doi.org/10.3390/min10090812
Brandt F, Klinkenberg M, Poonoosamy J, Bosbach D. Recrystallization and Uptake of 226Ra into Ba-Rich (Ba,Sr)SO4 Solid Solutions. Minerals. 2020; 10(9):812. https://doi.org/10.3390/min10090812
Chicago/Turabian StyleBrandt, Felix, Martina Klinkenberg, Jenna Poonoosamy, and Dirk Bosbach. 2020. "Recrystallization and Uptake of 226Ra into Ba-Rich (Ba,Sr)SO4 Solid Solutions" Minerals 10, no. 9: 812. https://doi.org/10.3390/min10090812
APA StyleBrandt, F., Klinkenberg, M., Poonoosamy, J., & Bosbach, D. (2020). Recrystallization and Uptake of 226Ra into Ba-Rich (Ba,Sr)SO4 Solid Solutions. Minerals, 10(9), 812. https://doi.org/10.3390/min10090812