Geochemical Characteristics and Environmental Risk Assessment of Heavy Metals in Weathering Profiles of Alkali-enriched Porphyry in Central Yunnan
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摘要:
中国西南地区发育大规模富碱斑岩带，通常具有重金属高背景值的特征，岩石风化是重金属的重要来源，土壤重金属污染是全球性关注的热点问题。在云南水热条件充足、成土作用强烈的条件下，为了查清富碱斑岩成土过程中重金属元素地球化学行为特征以及可能带来的一系列生态环境问题。本文选择滇中姚安富碱斑岩岩石风化剖面为研究对象，采用电感耦合等离子体质谱/发射光谱法（ICP-MS/OES）、原子荧光光谱法（AFS）、X射线荧光光谱法（XRF）、容量法等方法测定岩石和土壤样品中As、Cd、Cr、Cu、Hg、Ni、Pb、Zn、Al2O3、TFe2O3、CaO、Na2O、K2O、MgO、SiO2、有机碳等主微量元素含量和pH值，利用多元统计学方法和质量迁移系数研究风化剖面中重金属元素分布特征、迁移富集规律及影响因素，探讨富碱斑岩风化成土过程中重金属地球化学特征，揭示重金属元素迁移富集机制及可能带来的生态环境问题。结果表明：①富碱斑岩各风化层元素分布特征继承了基岩的特征，在风化成土过程中，As、Cr、Cu、Hg和Cd、Pb、Zn具有相似的地球化学行为，相对于Ti，重金属迁移能力强弱顺序为：Cd＞Zn＞Pb＞Hg＞Cu＞As＞Ni＞Cr；②Cu、Cr、Ni、Hg受其自身化学性质和脱硅富铝铁作用的影响，随风化最终富集于黏土矿物与Al、Fe氧化物/氢氧化物中，As与Fe、Al结合成难溶性的化合物而显著富集，土壤层迁移系数均值为7.64，Cd、Pb、Zn在酸性和强淋溶条件下显著地淋失迁移，土壤层迁移系数均值分别为−0.67、−0.45、−0.59。与大部分铅锌矿区相似，As受富铝铁作用影响原地次生富集，Cd、Pb、Zn受自身活泼的化学性质和pH影响大量淋失；③研究区土壤生态环境可能存在As、Pb污染的风险，Pb的大量淋失可能随地表径流迁入蜻岭河，应加强对富碱斑岩上覆土壤中As、Pb和流经富碱斑岩区河流中Pb、Zn的监测。
Abstract:BACKGROUND The contents of many heavy metals in soil in many areas of southwest China are much higher than the national soil background value, and related studies show that most heavy metals in soil are in a state of “high background and low activity”, which is closely related to the special geological process in the area. Most scholars have concentrated more on the weathering process and post-weathering heavy metals of granite, basalt, carbonate rocks and other geological bodies with high background value of heavy metals in southwest China. However, alkali-enriched porphyry also has the characteristics of high background value of heavy metals, and the geochemical behavior characteristics of heavy metals in the weathering process of alkali-enriched porphyry are less studied. The ecological and environmental effects of heavy metal element migration and transformation during weathering are still unclear. There is a large-scale alkali-enriched porphyry belt located in southwest China. Most of the alkali-enriched porphyry areas have precious metals such as gold and silver, and polymetallic deposits such as copper, lead and zinc. Therefore, soil in alkali-enriched porphyry areas usually has the characteristic of high background value of heavy metals.
OBJECTIVES For identifying geochemical characteristics of heavy metal elements and a series of ecological and environmental problems during the soil-forming process of alkali-enriched porphyry, to provide a scientific basis for the prevention and control of heavy metal pollution in alkali-enriched porphyry areas and rational planning of agricultural planting.
METHODS For sufficient hydrothermal conditions and strong soil-forming in Yunnan Province, a rock weathering profile of Yao’an alkali-enriched porphyry in central Yunnan Province was selected as the research object. The contents of As, Cd, Cr, Cu, Hg, Ni, Pb, Zn, Al2O3, TFe2O3, CaO, Na2O, K2O, MgO, SiO2, organic carbon and pH in rock/soil samples were determined by inductively coupled plasma-mass spectrometry/optimal emission spectrometry (ICP-MS/OES), atomic fluorescence spectrometry (AFS), X-ray fluorescence spectrometry (XRF) and volumetric method. Multivariate statistics method and mass migration coefficient were used to study the distribution characteristics, migration and enrichment rules of heavy metal elements in the weathering profile, as well as the factors affecting the migration and enrichment of heavy metals.
RESULTS Based on the analysis of the content and distribution characteristics of eight heavy metals in the weathering profile of Yao’an alkali-enriched porphyry, the migration and enrichment mechanism of heavy metals during the weathering process was identified, and the environmental risk assessment of the surface soil in the area was carried out. (1) In the weathering profile, all the weathering strata have the same source as the bedrock material, and there is no exogenous addition. Different degrees of desiliconization and aluminum-iron enrichment occur in the whole weathering process, especially in the surface layer. In the bottom-up evolution process, all of the heavy metal elements except Cd show an overall trend of increasing content. As, Cr, Cu, Hg and Ni are enriched to different degrees during weathering, while Cd, Pb and Zn are leaching out. The order of heavy metal migration capacity from strong to weak is Cd>Zn>Pb>Hg>Cu>As>Ni>Cr. As, Cr, Cu, and Hg have similar geochemical behavior, as do Cd, Pb, and Zn. (2) Cd, Pb and Zn occur mainly in feldspar minerals and lead-zinc metallic minerals and exhibit the characteristics of migration and leaching under acidic and strong leaching conditions. Although the bedrock is obviously deficient in Cu, Cr, Ni and Hg, it is eventually enriched in-situ in clay minerals and Al and Fe oxides/hydroxides with weathering due to its own chemical properties and the effect of desilication to enrich aluminum and iron. The enrichment of As is mainly controlled by aluminum-Fe enrichment, and the strong aluminum-Fe enrichment in the study area results in the in-situ secondary enrichment of As. (3) The soil ecological environment in the study area may be polluted by As and Pb due to the high content of Pb in the bedrock and the effect of aluminum-iron enrichment.
CONCLUSIONS The risk of As and Pb pollution may exist in the soil ecological environment of the study area, and a large amount of Pb leaching may migrate into the Dragonling River with surface runoff. It is necessary to strengthen the monitoring of heavy metals such as As and Pb in the overlying soil of alkali-enriched porphyry and heavy metals such as Pb and Zn in the rivers around alkali-enriched porphyry so as to ensure ecological safety.
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表 1 富碱斑岩风化剖面中微量元素组成与理化指标
Table 1. Composition and physical and chemical indexes of trace elements in weathering profile of alkali-rich porphyry.
风化层
划分样品编号 深度
(cm)As
(mg/kg)Cd
（mg/kg）Cr
（mg/kg）Cu
（mg/kg）Hg
（mg/kg）Ni
（mg/kg）Pb
（mg/kg）Zn
（mg/kg）Zr
（mg/kg）Ti
（mg/kg）SOM
（%）CIA
（%）全风化层 YPM01-01 30 71.70 0.16 142.00 52.40 0.05 60.40 241.00 147.00 756.00 6076 0.40 93.04 YPM01-02 90 70.10 0.16 128.00 41.00 0.05 50.60 201.00 119.00 754.00 5896 0.53 90.50 半风化层 YPM01-03 200 74.10 0.16 134.00 39.50 0.04 51.10 204.00 141.00 735.00 5681 0.34 91.69 YPM01-04 270 63.90 0.10 105.00 18.30 0.03 48.40 168.00 152.00 957.00 6398 0.28 81.18 YPM01-05 320 6.81 0.09 58.40 12.50 0.02 60.00 108.00 192.00 827.00 4252 0.17 72.82 YPM01-06 370 7.45 0.08 53.70 11.90 0.01 46.20 123.00 145.00 899.00 4316 0.14 64.20 过渡层 YPM01-07 440 5.12 0.20 52.30 17.30 0.01 51.40 117.00 171.00 894.00 3813 0.16 62.55 YPM01-08 530 2.25 0.21 61.20 21.70 ☆ 49.40 108.00 183.00 891.00 3471 0.14 59.96 YPM01-09 700 3.19 0.12 57.80 15.90 ☆ 52.10 84.00 196.00 833.00 3817 0.10 58.65 YPM01-10 820 3.34 0.18 59.90 17.60 0.005 50.60 88.80 182.00 854.00 3960 0.07 58.88 YPM01-11 900 1.40 0.09 79.70 13.70 0.01 59.80 93.40 142.00 864.00 3639 0.24 55.56 基岩 YPM01-12 1000 2.41 0.14 10.20 8.36 0.01 10.40 118.00 94.40 584.00 1757 0.12 46.08 UCC 1.50 0.098 35.85 25.00 0.0123 20.44 20.17 71.00 190.00 3000 △ △ 碱性侵入岩区表层土壤 5.10 0.11 32.00 13.00 0.06 13.00 36.00 65.00 311.00 3571 2.14 △ 云南省表层土壤 10.60 0.27 91.00 40.00 0.07 38.00 39.00 96.00 336.00 6193 2.48 △ 注：“△”表示低于检测限，“☆”表示无此数据，UCC数据来源于文献[26]，碱性侵入岩区表层、深层土壤数据来源于文献[27]。 
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表 2 风化剖面重金属元素迁移系数皮尔逊相关性特征
Table 2. Pearson correlation characteristics of heavy metal migration coefficient in weathering profile.
元素 As Cd Cr Cu Hg Ni Pb Zn As 1 Cd 0.422 1 Cr 0.634** 0.538 1 Cu 0.603* 0.175 0.594* 1 Hg 0.818** −0.220 0.364 0.529 1 Ni −0.610* −0.119 0.174 −0.246 −0.652* 1 Pb 0.137 0.639* −0.365 0.341 0.477 −0.663* 1 Zn −0.889** 0.680* −0.661* −0.349 −0.722** 0.444 0.101 1 注：“**”表示在p=0.01水平上显著；“*”表示在p=0.05水平上显著；n=12。
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表 3 风化剖面重金属元素与其他指标的皮尔逊相关性特征
Table 3. Pearson correlation characteristics of heavy metal elements and other indicators in weathering profile.
指标 As Cd Cr Cu Hg Ni Pb Zn SiO2 −0.895** −0.211 −0.973** −0.942** −0.874** −0.542 −0.872** 0.094 Al2O3 0.938** 0.055 0.925** 0.851** 0.929** 0.447 0.907** −0.145 TFe2O3 0.888** 0.155 0.907** 0.922** 0.929** 0.394 0.912** −0.260 MgO −0.684* −0.240 −0.439 −0.615* −0.675* 0.432 −0.782** 0.758** CaO −0.338 0.021 −0.588* −0.376 −0.281 −0.899** −0.236 −0.581* Na2O −0.879** −0.033 −0.899** −0.805** −0.871** −0.546 −0.832** −0.001 K2O −0.975** −0.086 −0.884** −0.871** −0.975** −0.213 −0.967** 0.375 SOM 0.871** 0.043 0.864** 0.816** 0.929** 0.283 0.860** −0.468 CIA 0.931** 0.054 0.926** 0.850** 0.921** 0.469 0.895** −0.117 Si/(Al+Fe) −0.876** −0.071 −0.939** −0.835** −0.866** −0.606* −0.833** 0.004 注：“**”表示在p=0.01水平上显著； “*”表示在p=0.05水平上显著； n=12。
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