天然镭同位素富集和测定方法及对河口混合过程的示踪研究
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摘要
河口是海洋初级生产力最高的区域,河口水体停留时间和地下水排放(SGD)通量对河口生态系统具有重要影响。天然镭同位素是研究河口过程的良好示踪工具,在滨岸海洋学研究中发挥着重要作用。分析河口地区各种镭同位素的比活度水平及分布特征,并以之为示踪剂进行水体停留时间和地下水排放通量的计算,是深入研究河口水体混合过程的一种十分有效的方法,可为认识河口地区物质的来源归宿、收支平衡和水体更新能力提供新的视角,为制定合理的生态环境保护措施提供重要的科学依据。
本研究首先制备了镭同位素的富集材料—“奥齐”丙烯腈型锰纤维,并应用同步延时计数器(RaDeCC)、γ能谱仪、氡射气闪烁计数器、RAD7测氡仪等仪器对各种镭同位素进行测定,着重研究并建立了RAD测氡仪的实验室校正体系;以此为基础,将辽河口、长江口、黄河口及其邻近海域作为研究区域,分析了研究海域水体中各种天然镭同位素的放射性比活度水平及其分布规律,并利用“镭同位素表观年龄”模型计算了河口水体的停留时间及运移速率,利用~(226)Ra“质量平衡模型”计算了黄河口海底地下水排放(SGD)的通量,评价了SGD对陆源物质向海输送的贡献。
本研究获得的主要结论如下:
1)研究制备了“奥齐”丙烯腈型锰纤维,经实验证明是一种优异的镭同位素富集材料。其制备流程简单,反应速度快,且反应节点容易判断。该纤维的各种镭同位素本底值很低。当被富集的水样流速不超过2 L min-1时,纤维对镭同位素的富集效率稳定在95-100%之间,但当流速为2-4 L min-1时,富集效率有较为明显的下降,但仍可保持在90%以上。
2)建立了RAD7测氡仪的实验室校正体系,最多可同时校正6台仪器。与美国DURRIDGE公司标准校正体系、美国佛罗里达州立大学Hollow Ridge Cave校正体系进行互较,实验数据在±2%的误差范围内。
3)辽河口水体中的~(224)Ra和~(223)Ra随盐度变化呈不保守现象,在盐度为10和26的海域出现了同位素比活度高峰值,结合pH、DO、COD、石油烃、叶绿素、营养盐等参数分析发现,盐度10左右的海区镭同位素高峰值可能是悬浮颗粒物解吸造成,盐度26左右的海区镭同位素高峰值则可能是由滨岸咸水地下水排放等因素造成。辽河口水体的停留时间最大值出现在盐度为14左右的海域,达到8.34天。
4)长江口及近海海域的~(224)Ra的放射性比活度范围为0.42-101.75 dpm 100L~(-1),~(223)Ra的放射性比活度范围为0.13-4.39 dpm 100L~(-1),~(226)Ra的放射性比活度范围为5.62-12.91 dpm 100L~(-1),228Ra的放射性比活度范围为34.28-57.55 dpm 100L~(-1),呈近岸高、远岸低和低潮高、高潮低的时空分布特点。在离岸30 km的范围内,水体的停留时间约为18天;但在离岸约60 km处的水体,根据“镭同位素表观年龄”模型计算的水体停留时间却降低为6天左右并保持相对稳定。这一“反常现象”是受到高镭淡水水团影响所致,根据盐度、水温、SPM的剖面分布以及悬浮颗粒物中的过剩~(210)Pb、~(234)Th的分布特征,推测该水团并非来自滨岸海底地下水排放(SGD),而是来自周边陆源径流。
5)黄河口及邻近海域水体中~(224)Ra、~(223)Ra、~(226)Ra的比活度范围分别为4.17-140.35 dpm 100L~(-1)、0.70-4.02 dpm 100L~(-1)、27.71-65.52 dpm 100L~(-1),各种镭同位素随盐度的分布均呈现“中间高、两端低”的不保守现象。根据“镭同位素表观年龄”模型计算的水体运移速率,发现9月份黄河水出口门后,大部分水体迅速右转,以5-7 km d~(-1)的流速向着东南方向流动,经过大约1周的时间到达莱州湾湾顶;另一部分水体向东北方向流动,以小于2 km d~(-1)的速度汇入渤海中央环流。该区域的海底地下水排放(SGD)通量为0.15-0.67 m~3 m~(-2) d~(-1),约为黄河径流量的3-13倍,由其携带入海的溶解铀和溶解无机氮的通量也显著高于黄河径流输送量,表明SGD是黄河口海区陆源物质入海的重要输送途径,对该海域物质的来源归宿、收支平衡具有不可忽略的影响。
Estuaries are the most productive natural habitats in the world. Water residence times and submarine groundwater discharge (SGD) variations directly influence the ecological conditions and production rates in estuaries. Natural radium isotopes have become increasingly recognized for their utility in examining mixing processes in the coastal ocean. The information obtained from radium tracers can be applied to understand the source and fate of estuarine substances from a new perspective, as well as to develop management strategies for controlling the supply of terrestrial substances to offshore areas and protect the coastal environment.
In this study,“AOQI”acrylic manganese fiber was prepared as preconcentration material for radium adsorption from water samples. Radium isotopes were measured by Radium Delayed Coincidence Counter, gamma spectrometer, Radon in line and RAD7. The lab calibration system for RAD7 was particularly established. In Liaohe estuary, Yangtze River estuary and Yellow River estuary, radium isotopes were measured and used as tracers to quantify water mixing processes. Water residence times and SGD flux were calculated via“Apparent Radium Ages Model”and“Mass balance Model”, respectively. Moreover, the contribution of SGD carried terrestrial material to the ocean was assessed.
The author would love to highlight the main results in this thesis as follow:
1)“AOQI”acrylic manganese fiber was an excellent material for radium preconcentrtion. It was very easy to prepare and had pretty low radium background which could be neglected. Its absorption efficiency was high and stable. About 95-100% radium would be collected when water flow rate was slower than 2 L min-1. When water flow rate was 2-4 L min-1, the absorption efficiency decreased, but still higher than 90%.
2) The RAD7 calibration system developed in this study was an air loop circulation system with a reproducibility of about±2%. The system could maintain 6 machines at the same time. The intercomparisons with Durridge Co. and Florida State University were performed which produced comparable results within an uncertainty of about±2%.
3) In Liaohe estuary, the distribution of ~(224)Ra and ~(223)Ra were not conservative along salinity. There were two peak activities at salinity 10 and 26. Combined with other parameters, such as pH, DO, COD, petroleum hydrocarbon, chlorophyll and nutrients, the peak at salinity 10 seemed to be caused by suspended particles desorption, and the one at salinity 26 was influenced by saline submarine groundwater discharge. The largest water residence time was 8.34 days which appeared at the area with salinity of 14.
4) In Yangtze River estuary, the activities of ~(224)Ra, ~(223)Ra, ~(226)Ra and 228Ra were 0.42-101.75 dpm 100L~(-1), 0.13-4.39 dpm 100L~(-1), 5.62-12.91 dpm 100L~(-1) and 34.28-57.55 dpm 100L~(-1), respectively. The highest activity was appeared at low tide near-shore area and vice versa. Within the first 30 km offshore, the water residence times gradually increased to 18 days. An anomalous low salinity point occurred at a distance of 60 km, and the water ages based on the“Apparent Age Model”decreased to about 6 days and were fairly constant until 140 km offshore. The distribution of salinity, water temperature, SPM concentration demonstrated that this anomaly was influenced by terrestrial runoff rather than benthic inputs from a submarine spring.
5) In Yellow River estuary, the activities of ~(224)Ra、~(223)Ra and ~(226)Ra were 4.17-140.35 dpm 100L~(-1), 0.70-4.02 dpm 100L~(-1) and 27.71-65.52 dpm 100L~(-1), respectively. All the radium isotopes were non-conservative versus salinity. In September, most of the Yellow River water turned right immediately after it discharged into the estuary. Under a flow rate of 5-7 km d~(-1), the diluted Yellow Rive water arrived at the top of Laizhou Bay in about one week. Small amount of river water directed to the Bohai Sea in the northeast under a lower flow rate of less than 2 km d~(-1). The SGD flux ranged from 0.15-0.67 m~3 m~(-2) d~(-1), which was about 3-13 times of Yellow River discharge. The SGD input of dissolved uranium and nutrients were significantly higher than their fluxes of Yellow River runoff.
本研究首先制备了镭同位素的富集材料—“奥齐”丙烯腈型锰纤维,并应用同步延时计数器(RaDeCC)、γ能谱仪、氡射气闪烁计数器、RAD7测氡仪等仪器对各种镭同位素进行测定,着重研究并建立了RAD测氡仪的实验室校正体系;以此为基础,将辽河口、长江口、黄河口及其邻近海域作为研究区域,分析了研究海域水体中各种天然镭同位素的放射性比活度水平及其分布规律,并利用“镭同位素表观年龄”模型计算了河口水体的停留时间及运移速率,利用~(226)Ra“质量平衡模型”计算了黄河口海底地下水排放(SGD)的通量,评价了SGD对陆源物质向海输送的贡献。
本研究获得的主要结论如下:
1)研究制备了“奥齐”丙烯腈型锰纤维,经实验证明是一种优异的镭同位素富集材料。其制备流程简单,反应速度快,且反应节点容易判断。该纤维的各种镭同位素本底值很低。当被富集的水样流速不超过2 L min-1时,纤维对镭同位素的富集效率稳定在95-100%之间,但当流速为2-4 L min-1时,富集效率有较为明显的下降,但仍可保持在90%以上。
2)建立了RAD7测氡仪的实验室校正体系,最多可同时校正6台仪器。与美国DURRIDGE公司标准校正体系、美国佛罗里达州立大学Hollow Ridge Cave校正体系进行互较,实验数据在±2%的误差范围内。
3)辽河口水体中的~(224)Ra和~(223)Ra随盐度变化呈不保守现象,在盐度为10和26的海域出现了同位素比活度高峰值,结合pH、DO、COD、石油烃、叶绿素、营养盐等参数分析发现,盐度10左右的海区镭同位素高峰值可能是悬浮颗粒物解吸造成,盐度26左右的海区镭同位素高峰值则可能是由滨岸咸水地下水排放等因素造成。辽河口水体的停留时间最大值出现在盐度为14左右的海域,达到8.34天。
4)长江口及近海海域的~(224)Ra的放射性比活度范围为0.42-101.75 dpm 100L~(-1),~(223)Ra的放射性比活度范围为0.13-4.39 dpm 100L~(-1),~(226)Ra的放射性比活度范围为5.62-12.91 dpm 100L~(-1),228Ra的放射性比活度范围为34.28-57.55 dpm 100L~(-1),呈近岸高、远岸低和低潮高、高潮低的时空分布特点。在离岸30 km的范围内,水体的停留时间约为18天;但在离岸约60 km处的水体,根据“镭同位素表观年龄”模型计算的水体停留时间却降低为6天左右并保持相对稳定。这一“反常现象”是受到高镭淡水水团影响所致,根据盐度、水温、SPM的剖面分布以及悬浮颗粒物中的过剩~(210)Pb、~(234)Th的分布特征,推测该水团并非来自滨岸海底地下水排放(SGD),而是来自周边陆源径流。
5)黄河口及邻近海域水体中~(224)Ra、~(223)Ra、~(226)Ra的比活度范围分别为4.17-140.35 dpm 100L~(-1)、0.70-4.02 dpm 100L~(-1)、27.71-65.52 dpm 100L~(-1),各种镭同位素随盐度的分布均呈现“中间高、两端低”的不保守现象。根据“镭同位素表观年龄”模型计算的水体运移速率,发现9月份黄河水出口门后,大部分水体迅速右转,以5-7 km d~(-1)的流速向着东南方向流动,经过大约1周的时间到达莱州湾湾顶;另一部分水体向东北方向流动,以小于2 km d~(-1)的速度汇入渤海中央环流。该区域的海底地下水排放(SGD)通量为0.15-0.67 m~3 m~(-2) d~(-1),约为黄河径流量的3-13倍,由其携带入海的溶解铀和溶解无机氮的通量也显著高于黄河径流输送量,表明SGD是黄河口海区陆源物质入海的重要输送途径,对该海域物质的来源归宿、收支平衡具有不可忽略的影响。
Estuaries are the most productive natural habitats in the world. Water residence times and submarine groundwater discharge (SGD) variations directly influence the ecological conditions and production rates in estuaries. Natural radium isotopes have become increasingly recognized for their utility in examining mixing processes in the coastal ocean. The information obtained from radium tracers can be applied to understand the source and fate of estuarine substances from a new perspective, as well as to develop management strategies for controlling the supply of terrestrial substances to offshore areas and protect the coastal environment.
In this study,“AOQI”acrylic manganese fiber was prepared as preconcentration material for radium adsorption from water samples. Radium isotopes were measured by Radium Delayed Coincidence Counter, gamma spectrometer, Radon in line and RAD7. The lab calibration system for RAD7 was particularly established. In Liaohe estuary, Yangtze River estuary and Yellow River estuary, radium isotopes were measured and used as tracers to quantify water mixing processes. Water residence times and SGD flux were calculated via“Apparent Radium Ages Model”and“Mass balance Model”, respectively. Moreover, the contribution of SGD carried terrestrial material to the ocean was assessed.
The author would love to highlight the main results in this thesis as follow:
1)“AOQI”acrylic manganese fiber was an excellent material for radium preconcentrtion. It was very easy to prepare and had pretty low radium background which could be neglected. Its absorption efficiency was high and stable. About 95-100% radium would be collected when water flow rate was slower than 2 L min-1. When water flow rate was 2-4 L min-1, the absorption efficiency decreased, but still higher than 90%.
2) The RAD7 calibration system developed in this study was an air loop circulation system with a reproducibility of about±2%. The system could maintain 6 machines at the same time. The intercomparisons with Durridge Co. and Florida State University were performed which produced comparable results within an uncertainty of about±2%.
3) In Liaohe estuary, the distribution of ~(224)Ra and ~(223)Ra were not conservative along salinity. There were two peak activities at salinity 10 and 26. Combined with other parameters, such as pH, DO, COD, petroleum hydrocarbon, chlorophyll and nutrients, the peak at salinity 10 seemed to be caused by suspended particles desorption, and the one at salinity 26 was influenced by saline submarine groundwater discharge. The largest water residence time was 8.34 days which appeared at the area with salinity of 14.
4) In Yangtze River estuary, the activities of ~(224)Ra, ~(223)Ra, ~(226)Ra and 228Ra were 0.42-101.75 dpm 100L~(-1), 0.13-4.39 dpm 100L~(-1), 5.62-12.91 dpm 100L~(-1) and 34.28-57.55 dpm 100L~(-1), respectively. The highest activity was appeared at low tide near-shore area and vice versa. Within the first 30 km offshore, the water residence times gradually increased to 18 days. An anomalous low salinity point occurred at a distance of 60 km, and the water ages based on the“Apparent Age Model”decreased to about 6 days and were fairly constant until 140 km offshore. The distribution of salinity, water temperature, SPM concentration demonstrated that this anomaly was influenced by terrestrial runoff rather than benthic inputs from a submarine spring.
5) In Yellow River estuary, the activities of ~(224)Ra、~(223)Ra and ~(226)Ra were 4.17-140.35 dpm 100L~(-1), 0.70-4.02 dpm 100L~(-1) and 27.71-65.52 dpm 100L~(-1), respectively. All the radium isotopes were non-conservative versus salinity. In September, most of the Yellow River water turned right immediately after it discharged into the estuary. Under a flow rate of 5-7 km d~(-1), the diluted Yellow Rive water arrived at the top of Laizhou Bay in about one week. Small amount of river water directed to the Bohai Sea in the northeast under a lower flow rate of less than 2 km d~(-1). The SGD flux ranged from 0.15-0.67 m~3 m~(-2) d~(-1), which was about 3-13 times of Yellow River discharge. The SGD input of dissolved uranium and nutrients were significantly higher than their fluxes of Yellow River runoff.
引文
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