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Abstract: In order to characterize the features of radium isotopes in estuaries of Tianjin, a continuous survey and sampling of typical estuaries were conducted from 2013 to 2017 in this study. The activities of natural radioactive radium isotopes (223Ra, 224Ra, and 228Ra) in groundwater and surface water were measured by the radium-delayed coincidence counting (RaDeCC) system. The non-conservative behavior of the radium isotopes was investigated under hydrogeochemical conditions and urbanization. The results indicated that in terms of horizontal distribution, the activities of radium in groundwater (Hangu, Tanggu, and Dagang) showed an upward trend from north to south and demonstrated a higher figure than surface water (Haihe River and Duliujian River). Concerning the vertical distribution, the activitives of radium at a 15 m burial depth was higher than that at a 30 m burial depth in all measurements. The activities of radium isotopes in the study area increased with the increase of total dissolved solids, and their desorption behavior on Fe-Mn oxides was constrained by the redox intensity. Different hydrogeological conditions resulted in variations in the vertical profile of radium activities. The activity of radium was regulated by seasonal variation and precipitation in groundwater and surface water. In addition, the rapid urbanization has caused a significant impact on the features of radium isotopes in typical estuaries of Tianjin. Meanwhile, radium isotopes can be applied to reflect the impact of urbanization on surface water-groundwater systems. Clarifying and cleverly utilizing the relationship between behavior of radium isotopes and urbanization will promote the development of the Tianjin Binhai New Area in a healthy way.
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Key words:
- estuary /
- radium isotope /
- total dissolved solids /
- ionic strength /
- urbanization
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Figure 1. The scope of the study area and sampling stations. HG: Hangu; TG: Tanggu; DG: Dagang; HH: Haihe River; DLJ: Duliujian River.
Figure 2. Horizontal distribution of 223Ra (a, b), 224Ra (c, d) and 228Ra (e, f) activities in groundwater (HG: Hangu; TG: Tanggu; DG: Dagang).
Figure 3. Horizontal distribution of 223Ra (a−c), 224Ra (d−f) and 228Ra (g−i) activities in surface water (HH: Haihe River; DLJ: Duliujian River).
Figure 4. Activity of 223Ra, 224Ra and 228Ra in surface water (Haihe River (a) and Duliujian River (b)) at each station.
Figure 5. Groundwater vertical distribution of 223Ra, 224Ra and 228Ra activities in spring (a−c) and autumn (d−f).
Figure 6. Different kinds of plots depicting 223Ra (a, b), 224Ra (c, d) and 228Ra (e, f) activities of groundwater (HG: Hangu; TG: Tanggu; DG: Dagang) in relationship with total dissolved solid (TDS) in spring and autumn.
Figure 7. Different kinds of plots depicting 223Ra (a−c), 224Ra (d−f) and 228Ra (g−i) activities of surface water (HH: Haihe River; DLJ: Duliujian River) in relationship with total dissolved solid (TDS) in spring, summer and autumn.
Figure 8. Different kinds of plots depicting 223Ra, 224Ra and 228Ra activities in relationship with
${{\rm {NO}}_3^{-}} $ (a, b) and${{\rm {SO}}_4^{2-}} $ (c, d) in spring and autumn.
Figure 9. Relationship between 224Ra/228Ra isotope activity ratio and precipitation (mm) under different seasonal variations in groundwater (a, b) and surface water (c, d).
Figure 10. Relationship between rapid urbanization and radium isotopes in Tianjin Binhai New Area. SGD: submarine groundwater discharge.
Table 1. Measurements of 223Ra, 224Ra and 228Ra in groundwater
Sample Depth/m Latitude Longitude 223Ra/(dpm·(100 L)−1) 224Ra/(dpm·(100 L)−1) 228Ra/(dpm·(100 L)−1) Spring Autumn Spring Autumn Spring Autumn HG1 15 39.21°N 117.63°E 3.18 1.07 35.22 21.92 23.61 35.97 HG3 15 39.18°N 117.66°E 0.28 0.57 26.97 41.07 3.61 40.31 HG4 15 39.17°N 117.67°E 0.13 − 31.30 − 11.12 − HG4 30 39.17°N 117.67°E 0.26 − 9.03 − 6.71 − HG5 15 39.16°N 117.67°E 5.61 17.78 383.21 503.87 201.48 332.40 HG6 15 39.15°N 117.69°E 5.68 − 631.97 − 374.02 − HG6 30 39.15°N 117.69°E 0.24 − 56.28 − 64.14 − HG7 15 39.15°N 117.70°E 9.93 2.44 612.76 95.93 231.90 236.06 TG1 15 38.93°N 117.67°E 10.53 − 209.42 − 425.16 − TG2 15 38.94°N 117.66°E 5.87 − 138.73 − 416.04 − TG3 15 38.95°N 117.65°E 102.94 − 618.67 − 488.19 − TG3 30 38.95°N 117.65°E 1.49 24.74 65.34 1936.98 36.57 32.61 TG4 15 38.95°N 117.63°E 22.99 − 885.81 − 310.46 − TG5 15 38.95°N 117.61°E 1.34 9.94 80.45 317.81 72.22 169.45 TG5 30 38.95°N 117.61°E 2.31 0.89 3384.80 104.72 1099.93 23.24 TG7 15 38.97°N 117.56°E 0.66 0.52 63.47 17.42 93.21 33.73 TG8 15 38.99°N 117.53°E 1.20 1.49 40.92 52.20 55.61 55.11 TG8 30 38.99°N 117.53°E 7.49 − 289.43 − 340.15 − TG9 15 39.00°N 117.47°E 1.68 0.11 104.48 25.38 66.16 69.78 DG1 15 38.64°N 117.38°E 38.41 12.80 976.90 448.77 809.54 236.07 DG1 30 38.64°N 117.38°E 3.51 0.01 132.69 11.68 100.23 13.61 DG2 15 38.64°N 117.40°E 113.35 40.24 2702.10 906.58 949.95 904.35 DG3 15 38.65°N 117.44°E 70.22 1.06 1383.59 71.15 623.95 456.40 DG4 15 38.66°N 117.47°E 64.15 66.05 1489.13 1563.82 471.53 928.50 DG4 30 38.66°N 117.47°E 3.12 2.79 86.04 111.23 65.22 318.54 DG5 15 38.66°N 117.49°E 321.64 61.40 3022.17 1814.50 1047.14 1063.86 DG5 30 38.66°N 117.49°E 2.74 4.45 58.27 126.65 63.36 573.35 DG6 15 38.66°N 117.51°E 356.12 61.55 3281.96 1846.62 1452.83 1810.29 DG7 30 38.66°N 117.52°E 357.64 1.59 3026.60 182.59 1100.73 198.41 DG7 15 38.66°N 117.52°E 2.48 15.92 198.73 947.32 332.17 1035.72 DG8 15 38.66°N 117.56°E 314.88 11.17 4276.96 214.62 2004.84 572.41 DG9 15 38.66°N 117.55°E 47.34 24.28 1671.79 552.71 639.33 825.89 DG9 30 38.66°N 117.55°E 10.32 4.51 314.65 173.82 415.58 495.18 DG10 15 38.67°N 117.54°E 91.89 18.79 2105.74 426.99 766.39 1060.53 Note: HG: Hangu; TG: Tanggu; DG: Dagang. − represents no data. 
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Table 2. Measurements of 223Ra, 224Ra and 228Ra in surface water
Station Latitude Longitude 223Ra/(dpm·(100 L)−1) 224Ra/(dpm·(100 L)−1) 228Ra/(dpm·(100 L)−1) Spring Summer Autumn Spring Summer Autumn Spring Summer Autumn HH1 39.13°N 117.20°E 0.24 0.31 0.39 7.06 10.16 7.64 11.39 15.15 7.41 HH2 39.10°N 117.24°E 0.34 0.36 0.38 4.55 8.76 6.25 8.95 13.56 7.53 HH3 39.08°N 117.29°E 0.38 0.29 0.43 6.92 9.04 8.57 10.75 24.95 9.59 HH4 39.05°N 117.51°E 0.11 0.29 0.41 5.20 10.43 8.04 14.07 10.45 9.12 HH5 38.99°N 117.51°E 0.46 0.73 0.70 17.05 17.35 12.20 50.68 35.65 34.67 HH6 38.98°N 117.58°E 0.79 0.54 0.84 17.10 18.30 14.56 59.69 58.07 37.85 HH7 38.99°N 117.71°E 2.13 2.34 2.03 40.43 50.07 45.02 193.13 156.77 188.08 DLJ1 38.84°N 117.30°E 2.02 2.49 1.13 51.75 50.62 23.09 52.11 53.61 41.17 DLJ2 38.88°N 117.21°E 2.79 1.95 1.35 56.38 46.00 31.80 53.48 41.84 39.58 DLJ3 38.91°N 117.18°E 2.08 2.14 1.34 60.20 49.91 25.85 50.85 51.42 37.98 DLJ4 38.99°N 117.09°E 1.59 1.46 1.22 42.58 30.92 27.64 32.28 20.32 27.61 DLJ5 39.00°N 117.06°E 1.95 0.93 0.98 43.54 45.48 22.39 33.34 38.84 22.57 DLJ6 39.03°N 116.98°E 2.25 1.54 0.72 56.04 42.10 20.46 44.32 31.06 19.46 DLJ7 39.05°N 116.92°E 1.08 1.55 0.66 33.07 31.75 15.81 33.85 29.92 18.99 Note: HH: Haihe River; DLJ: Duliujian River.
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Table 3. Measurements of chemical concentration parameters in groundwater in spring
Sample Depth/
mTDS/
(mg·L−1)K+/
(mg·L−1)Ca2+/
(mg·L−1)Na+/
(mg·L−1)Mg2+/
(mg·L−1)${{\rm {HCO}_3^-}} $/
(mg·L−1)${{\rm {SO}}_4^{2-}} $/
(mg·L−1)$ {{\rm {NO}}_3^-} $/
(mg·L−1)${\rm{Cl}}^- $/
(mg·L−1)HG1 15 15678 67 60 11613 197 1360 1250 0.92 1130 HG3 15 8824 82 43 4305 133 930 760 1.29 2570 HG4 15 6731 116 103 5434 284 553 118 0.52 123 HG4 30 4257 21 26 2998 62 558 232 0.25 360 HG5 15 34702 232 187 7602 357 362 2860 1.21 23100 HG6 15 23180 267 199 3057 343 412 4700 0.74 14200 HG6 30 14994 161 70 6949 254 89 740 0.67 6730 HG7 15 19313 205 113 2166 314 585 3230 0.62 12700 TG1 15 79654 481 370 9682 382 533 14200 6.60 54000 TG2 15 52203 354 351 8791 399 56 6550 1.76 35700 TG3 15 104833 490 303 5048 397 293 14000 2.21 84300 TG3 30 121341 532 299 15089 398 322 13700 2.36 91000 TG4 15 22963 351 69 2017 354 661 4110 0.81 15400 TG5 15 58255 249 339 12475 389 − 3900 3.09 40900 TG5 30 46801 254 279 10395 382 10 2580 1.40 32900 TG7 15 10776 35 46 8523 103 484 870 0.25 714 TG8 15 4665 19 44 2849 68 723 520 8.37 433 TG8 30 22007 141 105 15683 232 551 412 3.50 4880 TG9 15 6103 35 48 3978 75 755 462 1.97 748 DG1 15 26912 192 97 6682 343 841 855 1.86 17900 DG1 30 16949 117 21 3116 339 300 855 0.93 12200 DG2 15 44082 299 181 8850 386 474 2490 1.29 31400 DG3 15 28403 254 112 4691 376 508 2460 1.06 20000 DG4 15 43380 274 213 8939 355 218 4080 0.90 29300 DG4 30 17297 65 53 4542 334 181 1420 1.00 10700 DG5 15 70040 343 313 14673 379 231 6100 1.26 48000 DG5 30 20207 75 134 6355 310 72 1460 0.87 11800 DG6 15 57951 344 311 12980 373 303 4640 1.23 39000 DG7 30 59115 314 301 13010 377 273 3340 1.30 41500 DG7 15 23947 156 92 10128 318 82 970 0.97 12200 DG8 15 80300 395 264 16159 374 456 4650 1.52 58000 DG9 15 72836 395 234 14911 373 122 6000 1.44 50800 DG9 30 20547 239 116 3800 320 62 1410 0.83 14600 DG10 15 43826 324 198 10930 367 384 4420 2.99 27200 Note: − represents no data. TDS: total dissolved solids.
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Table 4. Measurements of chemical concentration parameters in groundwater in autumn
Sample Depth/
mTDS/
(mg·L−1)K+/
(mg·L−1)Ca2+/
(mg·L−1)Na+/
(mg·L−1)Mg2+/
(mg·L−1)${{\rm {HCO}_3^-}} $/
(mg·L−1)${{\rm {SO}}_4^{2-}} $/
(mg·L−1)$ {{\rm {NO}}_3^-} $/
(mg·L−1)${\rm{Cl} }^- $/
(mg·L−1)HG1 15 4691 47 26 1274 228 837 1005 0.52 1274 HG3 15 6997 66 46 2103 172 645 834 1.26 3130 HG5 15 9657 76 6 2848 267 231 1627 1.15 4600 HG7 15 26654 181 50 7687 909 249 1698 0.56 15880 TG3 15 73568 1699 847 41400 8015 31 1814 2.36 19760 TG3 30 164712 1721 832 44220 8546 176 12034 2.46 97180 TG5 15 70196 268 670 19520 3749 70 3376 2.24 42540 TG5 30 80081 280 757 20710 4257 66 4870 1.40 49140 TG7 15 1935 24 27 549 80 308 333 1.03 612 TG8 15 2015 11 43 645 41 506 231 4.64 533 TG9 15 2470 24 26 730 82 376 422 1.88 808 DG1 15 8701 50 63 2378 365 181 272 1.76 5391 DG1 30 1512 39 32 376 30 37 431 0.83 568 DG2 15 64348 337 211 17110 2960 113 2836 1.19 40780 DG3 15 46939 256 67 12490 2066 149 2660 0.99 29250 DG4 15 57208 75 196 16340 1661 61 4074 0.85 34800 DG4 30 53374 173 49 14480 1848 42 2541 1.00 34240 DG5 15 86353 380 423 22250 3193 59 6718 1.16 53330 DG5 30 67421 309 371 17490 2447 40 4004 0.85 42760 DG6 15 84240 402 583 22260 2173 77 5094 1.22 53650 DG7 30 84254 430 553 22060 2996 74 3700 1.29 54440 DG7 15 30442 205 45 8433 1055 353 − 0.87 20350 DG8 15 33488 281 475 8621 818 48 3933 1.44 19310 DG9 15 94240 680 8 25690 3030 49 7012 1.50 57770 DG9 30 38044 232 145 10350 1107 29 1890 0.93 24290 DG10 15 66001 446 220 17170 2350 141 5510 3.01 40160 Note: − represents no data. TDS: total dissolved solids.
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Table 5. Stratigraphic division of groundwater (Hangu (HG), Tanggu (TG) and Dagang (DG)) profiles
Study
areaLayer bottom
elevation/mComposition of sediments HG −9.6 sand silty sand layer HG −18.0 silt layer HG −19.0 silt layer HG −21.0 clay silty sand layer TG −18.6 clay silty sand layer TG −19.2 shell sand layer TG −20.3 clay silty sand layer TG −23.0 silt layer DG −10.0 clay silty sand layer and fine sand layer DG −16.7 clay silty sand layer DG −30.2 clay silty sand layer
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