赣南稀土矿区土壤环境特征及稀土金属地球化学行为研究
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摘要
稀土资源的开发利用与其他资源一样,具有人类深度干扰、环境污染突出、生态严重恶化等特征,且稀土资源开发的污染问题一直被其应用价值特别是在农业方面的有益作用所掩盖,以至对稀土矿区生态环境问题的认识多停留在水土流失、植被破坏等表面现象上。目前针对稀土资源开发影响下对生态环境的影响研究相对比较零散,系统性不强,且较多集中在农用稀土进入土壤环境后稀土元素的地球化学行为等方面。本研究选取赣南三个稀土矿区——龙南高钇型稀土矿区、寻乌低钇低铕型稀土矿区和信丰中钇富铕型稀土矿区作为研究对象,结合野外取样、实验室模拟分析等方法,研究了赣南稀土矿区和稀土金属地球化学行为,得到如下结果。
(1)赣南典型稀土矿区土壤肥力和稀土金属污染特征。
矿区和矿区下游土壤综合肥力均比较低下,其中矿区土壤综合肥力为Ⅲ级(差),矿区下游土壤综合肥力为Ⅱ级(一般)；各稀土矿区土壤均呈酸性或弱酸性,有机质含量较低,土壤中盐基性离子淋失严重,阳离子交换量随着土壤酸性增强而降低；营养元素流失严重,氮磷钾在矿区和矿区下游土壤环境中处于缺乏状态,氮磷钾有效性较低；土壤综合肥力与开采历史呈现时间累积效应。
稀土矿区土壤环境中稀土金属含量均比较高,土壤稀土金属污染较严重。矿区土壤环境中稀土金属全量与稀土矿区开采历史、稀土矿区的开采状况有关系,如信丰稀土矿区开采历史短,矿区土壤环境中稀土金属全量最高；稀土金属有效性较高,稀土金属具有较高的活性。开采历史越短的矿区,其矿区和矿区下游土壤环境稀土金属有效性越高。
(2)稀土矿区水土环境酸化和稀土金属在垂直剖面方向分布的时间效应。
矿区土壤受稀土资源开发影响较大,土壤酸性较强,其中A层土壤酸化严重,到2011年10月,矿区土壤达到强酸性,土壤酸化现象极为严重,B层土壤酸性亦较强,酸化趋势比较明显,但C层土壤呈微弱减低趋势,呈弱酸性状态；矿区下游土壤A、B、C层酸化均比较严重,酸化程度是一个由表及里的过程,即A层酸化最严重(2011年快达到强酸性),B、C层次之；相比土壤环境,研究区水体pH值变化不明显。
矿区土壤环境中稀土全量和有效态稀土含量均极高,A、B层稀土全量逐年减少,稀土金属向低海拔区域和垂直方向发生迁移,C层土壤环境中稀土全量相对稳定,土壤A层中有效态稀土含量表现为逐年上升状态,但在同一年的4月(雨季)要比10月(旱季)要高；土壤B、C层中则维持在相对高值的状态；稀土金属在稀土矿区下游土壤环境中具有非常明显的表聚性,即土壤A层稀土金属增加明显,B层次之,C层微弱增加,有效态稀土金属含量与稀土全量具有类似特征。
(3)稀土酸性废水对土壤理化性质变化、营养元素含量和有效性以及稀土金属形态转化、累积迁移和有效性的影响。
稀土酸性废水的输入,胁迫土壤中稀土金属发生形态上的转化,使稀土金属有强烈向活性态稀土形态转化的趋势,活性态稀土金属随水力搬运作用和淋滤液淋出发生水平方向和垂直方向上的迁移,稀土金属向矿区下游区域扩散、吸附、累积,导致残渣态稀土金属含量和稀土全量降低以及稀土金属污染扩散。
(4)模拟酸雨及稀土金属污染对稀土矿区土壤酸化、土壤酶活性以及对稀土金属活化、形态转化、迁移累积影响。
不同酸碱度的模拟酸雨对稀土矿区土壤pH值、稀土淋失量及其化学形态转化的影响各不相同。模拟酸雨酸性越强,土壤酸化越严重,稀土淋出量越多,同时可能促进土壤中稀土形态之间的转化。
稀土尾矿经模拟酸雨淋溶后,土壤酸化严重,酸雨酸性越强,土壤酸化越严重；菜园土经稀土La、Ce单一和复合污染后,土壤酸化不明显,但经稀土尾矿淋出液污染后土壤酸化严重。土壤脲酶活性变化符合稀土金属“低促高抑”的生态效应；不同处理培养下土壤脲酶活性的抑制率表现为：尾矿稀土淋出液污染>稀土La、Ce复合污染>稀土Ce单一污染>稀土La单一污染。过氧化氢酶活性则表现为先抑制后轻微促进,不同处理培养下土壤脲酶活性的抑制率表现为：尾矿稀土淋出液污染>稀土La. Ce复合污染>稀土La单一污染>稀土Ce单一污染；土壤脲酶对稀土污染更为敏感。
综上所述,赣南典型稀土矿区土壤综合肥力低下,营养元素流失和稀土金属污染均比较严重,并不同程度地呈现时间累积效应；稀土金属含量及其有效性较高,极易通过土壤-植物、水土流失等途径进入食物链,造成污染扩散,存在较大的生态风险；稀土酸性废水和酸雨对稀土矿区土壤环境影响较大,可促进土壤酸化、理化性质变化、营养元素流失、土壤酶活性变化以及稀土金属活化溶出和形态转化,对区域生态环境的负面影响较大。
The development and utilization of rare earth, as other resources, has the characteristics of grievous human interference, prominent environmental pollution, deteriorated ecological seriously, etc. Moreover, the ecological problems caused by rare earth resources development were concealed by its application value especially in agriculture, and the comprehension about the entironment of rare earth mining area was always rested on superficial phenomena such as soil erosion, vegetation deterioration, etc. At present, the study on the ecological environment of rare earth for the influence of rare earth resources development is relatively fragmented and not systemic, in addition, mainly focuses on the geochemical behaviors of rare earth in agriculture after its entering into the soil environment. Three representative rare earth mining area (rich yttrium rare earth style mining area in Longnan, low yttrium and low europium style rare earth mining area in Xunwu, and middle yttrium and rich europium style rare earth mining area in Xinfeng) in Jiangxi Province, China, were chosen as study objects, combined with field sampling, laboratory simulation analysis method, the characteristics of soil environment and geochemical behaviors of rare earth metals were researched. The main conclusions could be drawn as follows:
(1) Characteristics of soil fertility and rare earth metals contamination of representative rare earth mining areas in Gannan region. Soil comprehensive fertility in the mining area and its downstream were all low, soil comprehensive fertility in mining area was rank III (Barren), and rank II (medium) of its downstream. The soil of all rare earth mining area presented acid or faintly acid; the content of soil organic matter in mining area and its downstream were low; the base saturation ions ran off seriously, the cation exchange capacity reduced with the increase of soil acidity; nutrient elements in soil was washed away partly, the content of NPK in mining area and its downstream was in short condition, and the availability of nutrient elements was low. The soil comprehensive fertility presented time effect appearance with the history of exploitation of rare earth mine.
The rare earth content in the soil environment of rare earth mining area was high, rare earth metals pollution in soil was serious. The total content of rare earth in soil was connected with time and conditions of exploitation, for instance, the exploitation time of Xinfeng rare earth mining area was short, the total content of rare earth in soil environment was highest. Rare earth metals in the soil environment of rare earth mining area had high bioavailability. The bioavailability of rare earth metals in the soil environment in rare earth mine of shorten exploitation history was more higher.
(2) Time effect about acidification of soil and water environment and rare earth metal distribution in the vertical profiles of the soil in rare earth mining area. Soil environment of mining area influenced greatly by rare earth resource exploitation, soil acidity was relative stronger, soil acidification of layer A was greatest, it's strong acidic until October2011; soil acidification of layer B was also rather strong, and had obvious trend of acidification; but soil acidification of layer C was weak acidic, and had weak trend of acidification. Soil of layer A, B and C in downstream of mining area all acidified seriously, the acidification was a process of from surface to inner, namely, layer A was most seriously(attained to strong acidic), layer B and C took second place. Compared with soil environment, the change of water body pH was not marked.
In soil environment of rare earth mining area, the contents of total rare earth and rare earth in bioavailability fractions were all extreme high, the content of rare earth in soil of layer A and B decreased year after year, rare earth metals migrated to the area of low altitude and vertical direction, and relative steady in soil of layer C. The content of rare earth in bioavailability fraction was in a state of increasing year by year, but it's higher in April (rainy season) than in October (dry season) of the same year, however, in soil of layer B and C, kept in a statue of high value relatively. Rare earth metals in soil environment of downstream in mining area had an obvious characteristic of superficial conglomeration, viz. the content of rare earth metals in soil of layer A increased obviously, layer B took the second place, and raised faintly in layer C, so as to rare earth in bioavailability fractions.
(3) Effect of rare earth acid mine drainage on the changes of soil physicochemical properties, content and availability of nutrient elements and transformation of fractions, accumulation, migration and availability of rare earth metals. Inputting of rare earth acid mine drainage could stress the transformation of fractions of rare earth metals, caused rare earth transform intensely to activity fractions, and rare earth metals in activity fractions migrated to horizontal and vertical direction by transportation of hydraulic power and eluviation of rare earth acid mine, rare earth metals occurred diffusion, adsorption, migration and accumulation from mining area to downstream of mining area, ultimately, brought about reduction of the content of rare earth in residual fraction and the total content of rare earth metals, and spreading of rare earth metals contamination.
(4) Effect of simulated acid rain and rare earth metals pollution on soil acidification, soil enzyme activities and activation, transformation of fraction, migration and accumulation of rare earth metals in soil environment of rare earth mining area. Simulated acid rain of different pH value had various effects on soil acidification and leaching content, the stronger the acidity of simulated acid rain, the severer the soil acidification, the greater the amount of rare earth leaching out. During the leaching out process, it might exist fraction transformation of rare earth metals.
After leached by simulated acid rain, tailings acidized seriously, the stronger acidity of simulated acid rain, the more serious of soil acidification. After incubated by single and combined contamination of La and Ce, vegetable soil pH changed unconspicuously, but for rare earth leachate, it's serious. The change of urease activity accorded with hormesis effect of RE. Treated with different incubation solution, the inhibition level of urease showed the order respectively of RE leachate> La+Ce> Ce> La. Accordingly, catalase activity was inhibited, and then promoted slightly. The inhibition level of urease showed the order respectively of RE leachate> La+Ce> La> Ce. Urease was more sensitive to RE contamination than catalase.
Generally, soil comprehensive fertility in representative rare earth mining area of Gannan region was infertile, the phenomena of nutrient element losing and rare earth metals pollution were all serious, simultaneously, which presented time accumulation effect in some degree. The content and availability of rare earth were high, rare earth acid mine drainage and acid rain could promote soil acidification, the change of physicochemical properties, losing of nutrient elements, the change of soil enzyme activities and transformation of fraction, leaching out of rare earth metals which were activated, and then brought about pollution diffusion of rare earth, existing potential ecological risk.
(1)赣南典型稀土矿区土壤肥力和稀土金属污染特征。
矿区和矿区下游土壤综合肥力均比较低下,其中矿区土壤综合肥力为Ⅲ级(差),矿区下游土壤综合肥力为Ⅱ级(一般)；各稀土矿区土壤均呈酸性或弱酸性,有机质含量较低,土壤中盐基性离子淋失严重,阳离子交换量随着土壤酸性增强而降低；营养元素流失严重,氮磷钾在矿区和矿区下游土壤环境中处于缺乏状态,氮磷钾有效性较低；土壤综合肥力与开采历史呈现时间累积效应。
稀土矿区土壤环境中稀土金属含量均比较高,土壤稀土金属污染较严重。矿区土壤环境中稀土金属全量与稀土矿区开采历史、稀土矿区的开采状况有关系,如信丰稀土矿区开采历史短,矿区土壤环境中稀土金属全量最高；稀土金属有效性较高,稀土金属具有较高的活性。开采历史越短的矿区,其矿区和矿区下游土壤环境稀土金属有效性越高。
(2)稀土矿区水土环境酸化和稀土金属在垂直剖面方向分布的时间效应。
矿区土壤受稀土资源开发影响较大,土壤酸性较强,其中A层土壤酸化严重,到2011年10月,矿区土壤达到强酸性,土壤酸化现象极为严重,B层土壤酸性亦较强,酸化趋势比较明显,但C层土壤呈微弱减低趋势,呈弱酸性状态；矿区下游土壤A、B、C层酸化均比较严重,酸化程度是一个由表及里的过程,即A层酸化最严重(2011年快达到强酸性),B、C层次之；相比土壤环境,研究区水体pH值变化不明显。
矿区土壤环境中稀土全量和有效态稀土含量均极高,A、B层稀土全量逐年减少,稀土金属向低海拔区域和垂直方向发生迁移,C层土壤环境中稀土全量相对稳定,土壤A层中有效态稀土含量表现为逐年上升状态,但在同一年的4月(雨季)要比10月(旱季)要高；土壤B、C层中则维持在相对高值的状态；稀土金属在稀土矿区下游土壤环境中具有非常明显的表聚性,即土壤A层稀土金属增加明显,B层次之,C层微弱增加,有效态稀土金属含量与稀土全量具有类似特征。
(3)稀土酸性废水对土壤理化性质变化、营养元素含量和有效性以及稀土金属形态转化、累积迁移和有效性的影响。
稀土酸性废水的输入,胁迫土壤中稀土金属发生形态上的转化,使稀土金属有强烈向活性态稀土形态转化的趋势,活性态稀土金属随水力搬运作用和淋滤液淋出发生水平方向和垂直方向上的迁移,稀土金属向矿区下游区域扩散、吸附、累积,导致残渣态稀土金属含量和稀土全量降低以及稀土金属污染扩散。
(4)模拟酸雨及稀土金属污染对稀土矿区土壤酸化、土壤酶活性以及对稀土金属活化、形态转化、迁移累积影响。
不同酸碱度的模拟酸雨对稀土矿区土壤pH值、稀土淋失量及其化学形态转化的影响各不相同。模拟酸雨酸性越强,土壤酸化越严重,稀土淋出量越多,同时可能促进土壤中稀土形态之间的转化。
稀土尾矿经模拟酸雨淋溶后,土壤酸化严重,酸雨酸性越强,土壤酸化越严重；菜园土经稀土La、Ce单一和复合污染后,土壤酸化不明显,但经稀土尾矿淋出液污染后土壤酸化严重。土壤脲酶活性变化符合稀土金属“低促高抑”的生态效应；不同处理培养下土壤脲酶活性的抑制率表现为：尾矿稀土淋出液污染>稀土La、Ce复合污染>稀土Ce单一污染>稀土La单一污染。过氧化氢酶活性则表现为先抑制后轻微促进,不同处理培养下土壤脲酶活性的抑制率表现为：尾矿稀土淋出液污染>稀土La. Ce复合污染>稀土La单一污染>稀土Ce单一污染；土壤脲酶对稀土污染更为敏感。
综上所述,赣南典型稀土矿区土壤综合肥力低下,营养元素流失和稀土金属污染均比较严重,并不同程度地呈现时间累积效应；稀土金属含量及其有效性较高,极易通过土壤-植物、水土流失等途径进入食物链,造成污染扩散,存在较大的生态风险；稀土酸性废水和酸雨对稀土矿区土壤环境影响较大,可促进土壤酸化、理化性质变化、营养元素流失、土壤酶活性变化以及稀土金属活化溶出和形态转化,对区域生态环境的负面影响较大。
The development and utilization of rare earth, as other resources, has the characteristics of grievous human interference, prominent environmental pollution, deteriorated ecological seriously, etc. Moreover, the ecological problems caused by rare earth resources development were concealed by its application value especially in agriculture, and the comprehension about the entironment of rare earth mining area was always rested on superficial phenomena such as soil erosion, vegetation deterioration, etc. At present, the study on the ecological environment of rare earth for the influence of rare earth resources development is relatively fragmented and not systemic, in addition, mainly focuses on the geochemical behaviors of rare earth in agriculture after its entering into the soil environment. Three representative rare earth mining area (rich yttrium rare earth style mining area in Longnan, low yttrium and low europium style rare earth mining area in Xunwu, and middle yttrium and rich europium style rare earth mining area in Xinfeng) in Jiangxi Province, China, were chosen as study objects, combined with field sampling, laboratory simulation analysis method, the characteristics of soil environment and geochemical behaviors of rare earth metals were researched. The main conclusions could be drawn as follows:
(1) Characteristics of soil fertility and rare earth metals contamination of representative rare earth mining areas in Gannan region. Soil comprehensive fertility in the mining area and its downstream were all low, soil comprehensive fertility in mining area was rank III (Barren), and rank II (medium) of its downstream. The soil of all rare earth mining area presented acid or faintly acid; the content of soil organic matter in mining area and its downstream were low; the base saturation ions ran off seriously, the cation exchange capacity reduced with the increase of soil acidity; nutrient elements in soil was washed away partly, the content of NPK in mining area and its downstream was in short condition, and the availability of nutrient elements was low. The soil comprehensive fertility presented time effect appearance with the history of exploitation of rare earth mine.
The rare earth content in the soil environment of rare earth mining area was high, rare earth metals pollution in soil was serious. The total content of rare earth in soil was connected with time and conditions of exploitation, for instance, the exploitation time of Xinfeng rare earth mining area was short, the total content of rare earth in soil environment was highest. Rare earth metals in the soil environment of rare earth mining area had high bioavailability. The bioavailability of rare earth metals in the soil environment in rare earth mine of shorten exploitation history was more higher.
(2) Time effect about acidification of soil and water environment and rare earth metal distribution in the vertical profiles of the soil in rare earth mining area. Soil environment of mining area influenced greatly by rare earth resource exploitation, soil acidity was relative stronger, soil acidification of layer A was greatest, it's strong acidic until October2011; soil acidification of layer B was also rather strong, and had obvious trend of acidification; but soil acidification of layer C was weak acidic, and had weak trend of acidification. Soil of layer A, B and C in downstream of mining area all acidified seriously, the acidification was a process of from surface to inner, namely, layer A was most seriously(attained to strong acidic), layer B and C took second place. Compared with soil environment, the change of water body pH was not marked.
In soil environment of rare earth mining area, the contents of total rare earth and rare earth in bioavailability fractions were all extreme high, the content of rare earth in soil of layer A and B decreased year after year, rare earth metals migrated to the area of low altitude and vertical direction, and relative steady in soil of layer C. The content of rare earth in bioavailability fraction was in a state of increasing year by year, but it's higher in April (rainy season) than in October (dry season) of the same year, however, in soil of layer B and C, kept in a statue of high value relatively. Rare earth metals in soil environment of downstream in mining area had an obvious characteristic of superficial conglomeration, viz. the content of rare earth metals in soil of layer A increased obviously, layer B took the second place, and raised faintly in layer C, so as to rare earth in bioavailability fractions.
(3) Effect of rare earth acid mine drainage on the changes of soil physicochemical properties, content and availability of nutrient elements and transformation of fractions, accumulation, migration and availability of rare earth metals. Inputting of rare earth acid mine drainage could stress the transformation of fractions of rare earth metals, caused rare earth transform intensely to activity fractions, and rare earth metals in activity fractions migrated to horizontal and vertical direction by transportation of hydraulic power and eluviation of rare earth acid mine, rare earth metals occurred diffusion, adsorption, migration and accumulation from mining area to downstream of mining area, ultimately, brought about reduction of the content of rare earth in residual fraction and the total content of rare earth metals, and spreading of rare earth metals contamination.
(4) Effect of simulated acid rain and rare earth metals pollution on soil acidification, soil enzyme activities and activation, transformation of fraction, migration and accumulation of rare earth metals in soil environment of rare earth mining area. Simulated acid rain of different pH value had various effects on soil acidification and leaching content, the stronger the acidity of simulated acid rain, the severer the soil acidification, the greater the amount of rare earth leaching out. During the leaching out process, it might exist fraction transformation of rare earth metals.
After leached by simulated acid rain, tailings acidized seriously, the stronger acidity of simulated acid rain, the more serious of soil acidification. After incubated by single and combined contamination of La and Ce, vegetable soil pH changed unconspicuously, but for rare earth leachate, it's serious. The change of urease activity accorded with hormesis effect of RE. Treated with different incubation solution, the inhibition level of urease showed the order respectively of RE leachate> La+Ce> Ce> La. Accordingly, catalase activity was inhibited, and then promoted slightly. The inhibition level of urease showed the order respectively of RE leachate> La+Ce> La> Ce. Urease was more sensitive to RE contamination than catalase.
Generally, soil comprehensive fertility in representative rare earth mining area of Gannan region was infertile, the phenomena of nutrient element losing and rare earth metals pollution were all serious, simultaneously, which presented time accumulation effect in some degree. The content and availability of rare earth were high, rare earth acid mine drainage and acid rain could promote soil acidification, the change of physicochemical properties, losing of nutrient elements, the change of soil enzyme activities and transformation of fraction, leaching out of rare earth metals which were activated, and then brought about pollution diffusion of rare earth, existing potential ecological risk.
引文
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