Migration and enrichment characteristics of heavy metals during the weathering and soil-forming process of carbonate rocks: A case study of typical areas in South China
SHI Xiao-xue1,2, SUN Qian-ying2, LU Yang2, WU Wen-cheng2, CHEN Wei-jie2
1. Department of Resources and Environment, Anhui University, Hefei 230601, China; 2. South China Institute of Environmental Sciences, Ministry of Ecology and Environment, Guangzhou 510655, China
Abstract：The weathered soil profiles were taken as the research objects from paddy and upland fields, which are typical agricultural lands in the carbonate rock regions of South China. The sources of soil heavy metals were traced via Pb isotope composition, and the vertical distribution and influencing factors of eight common types of heavy metals in the farmland soil profiles were systematically analyzed. The results revealed that the weathering of parent rocks was the main source of soil heavy metals in the study area, and the contents of heavy metals in the two profiles were found to be higher than the soil background value (0.056mg/kg). The enrichment of Cd tended to occur in the surface layer (0.49~2.15mg/kg) and the middle layer (0.75~1.87mg/kg) of the soil profiles, while that of the other elements tended to occur in the middle layer. The physicochemical properties and the mineral compositions of the soils, as well as the changes in the redox conditions exerted important impacts on the migration of heavy metals. The secondary enrichment of heavy metals in the soil profiles from the study area was attributed to the weathering process of carbonate rocks, while the impact of the leaching process on the migration and enrichment of heavy metals was more significant in the profile from the paddy field.
施小学, 孙乾迎, 卢阳, 吴文成, 陈伟杰. 碳酸盐岩风化成土过程重金属的迁移富集特征——以华南典型地区为例[J]. 中国环境科学, 2025, 45(4): 2063-2074.
SHI Xiao-xue, SUN Qian-ying, LU Yang, WU Wen-cheng, CHEN Wei-jie. Migration and enrichment characteristics of heavy metals during the weathering and soil-forming process of carbonate rocks: A case study of typical areas in South China. CHINA ENVIRONMENTAL SCIENCECE, 2025, 45(4): 2063-2074.
[1] Alloway B J.Heavy Metals in Soils:Trace metals and metalloids in soils and their bioavailability[M]. Environmental Pollution, 2013, 22:50. [2] Acosta J A, Martínez-Martínez S, Arocena J, et al. Accumulations of major and trace elements in particle size fractions of soils on eight different parent materials[J]. Geoderma, 2010,161:30-42. [3] Peng M, Zhao C, Ma H.Heavy metal and Pb isotopic compositions of soil and maize from a major agricultural area in Northeast China:Contamination assessment and source apportionment[J]. Journal of Geochemical Exploration, 2020,208:106403. [4] Gu Q,Yu T,Yang Z,et al.Prediction and risk assessment of five heavy metals in maize and peanut:A case study of Guangxi,China[J]. Environmental Toxicology and Pharmacology, 2019,70:103199. [5] Zhang L, McKinley J, Cooper M, et al. A regional soil and river sediment geochemical study in Baoshan area, Yunnan province, southwest China[J]. Journal of Geochemical Exploration, 2020, 217:106557. [6] Zhang L, McKinley J, Cooper M, et al. Transfer processes of potential toxic elements (PTE) between rock-soil systems and soil risk evaluation in the Baoshan area, Yunnan Province, Southwest China[J]. Applied Geochemistry, 2020,121:104712. [7] Yang Q, Yang Z, Filippelli G M, et al. Distribution and secondary enrichment of heavy metal elements in karstic soils with high geochemical background in Guangxi, China[J]. Chemical Geology, 2021,567:120081. [8] Liu Y, Xiao T, Ning Z, et al. High cadmium concentration in soil in the Three Gorges region:Geogenic source and potential bioavailability[J]. Applied Geochemistry, 2013,37:149-56. [9] 刘意章,肖唐付,朱建明.镉同位素及其环境示踪[J].地球与环境, 2015,43:687-696. Liu Y Z, Xiao T F, Zhu J M. Cadmium isotopes and environmental tracing[J]. Earth and Environment, 2015,43:687-696. [10] Wei X, Bai X, Wen X,et al.A large and overlooked Cd source in karst areas:The migration and origin of Cd during soil formation and erosion[J]. Science of the Total Environment, 2023,895:165126. [11] Wen Y, Li W, Yang Z, et al. Enrichment and source identification of Cd and other heavy metals in soils with high geochemical background in the karst region, Southwestern China[J]. Chemosphere, 2020,245:125620. [12] Wen Y, Li W, Yang Z,et al.Evaluation of various approaches to predict cadmium bioavailability to rice grown in soils with high geochemical background in the karst region, Southwestern China[J]. Environmental Pollution, 2020,258:113645. [13] Mu D, Zheng S, Lin D, et al. Derivation and validation of soil cadmium thresholds for the safe farmland production of vegetables in high geological background area[J]. Science of the Total Environment, 2023,873:162171. [14] Xiang M, Ma J, Cheng J, et al. Collaborative evaluation of heavy metal pollution of soil-crop system in the southeast of Yangtze River Delta, China[J]. Ecological Indicators, 2022,143:109412. [15] 肖蓓,王正海,申晋利,等.内蒙古钱家店铀矿区土壤-植物中重金属元素迁移富集特征[J].浙江大学学报(农业与生命科学版), 2022, 48:625-634. Xiao B, Wang Z H, Shen J L, et al. Migration and enrichment characteristics of heavy metal elements in soil plants of Qianjiadian Uranium Mining Area, Inner Mongolia[J]. Journal of Zhejiang University (Agriculture and Life Sciences Edition), 2022,48:625-634. [16] Temur S, Orhan H, Deli A.Geochemistry of the limestone of Mortas Formation and related terra rossa, Seydisehir, Konya, Turkey[J]. Geochemistry International, 2009,47:67-93. [17] Xiao J, Chen W, Wang L, et al. New strategy for exploring the accumulation of heavy metals in soils derived from different parent materials in the karst region of southwestern China[J]. Geoderma, 2022,417:115806. [18] Zhou Z, Wen H, Zhu C, et al. Effects of lithology and acid mine drainage on Cd concentration and isotope distribution in a large riverine system, Guangxi Province, South China[J]. Chemical Geology, 2023,634:121571. [19] 王振耀.广西龙州喀斯特地区碳酸盐岩风化成土作用中Cd元素的行为研究[D].南宁:南宁师范大学, 2020. Wang Z Y. Study on the behavior of Cd element in the weathering and soil formation of carbonate rocks in the karst area of Longzhou, Guangxi[D]. Nanning:Nanning Normal University, 2020. [20] 陈健.土壤pH测试方法及应用分析[J].化工设计通讯, 2020, 46:230,260. Chen J. Soil pH testing methods and application analysis[J]. Chemical Design Newsletter, 2020,46:230,260. [21] 叶钰,徐泽,阳冬秀,等.耕地土壤pH值和有机质含量空间分布特征及影响因素--以长沙县为例[J].湖南农业科学, 2024,3:37-40. Ye Y, Xu Z, Yang D X, et al. Spatial distribution characteristics and influencing factors of soil pH value and organic matter content in cultivated land:a case study of Changsha County[J]. Hunan Agricultural Science, 2024,3:37-40. [22] 孙福军,苗涵博,韩春兰,等.激光粒度仪法与湿筛-沉降法测定火山碎屑物发育土壤颗粒组成的比较[J].土壤通报, 2020,51:574-579. Sun F J, Miao H B, Han C L, et al. Comparison of laser particle size analyzer method and wet sieving sedimentation method for determining soil particle composition of volcanic debris development[J]. Soil Bulletin, 2020,5:15:574-579. [23] Feng J L, Pei L L, Zhu X, et al.Absolute accumulation and isotope fractionation of Si and Fe during dolomite weathering and terra rossa formation[J]. Chemical Geology, 2018,496:43-56. [24] Nesbitt H W.Mobility and fractionation of rare earth elements during weathering of a granodiorite[J]. Nature, 1979,279:206. [25] Song C, Ji H, Beckford H O, et al. Assessment of chemical weathering and physical erosion along a hillslope, southwest China[J]. CATENA, 2019,182:104133. [26] 文宇博.广西岩溶地质高背景地区土壤重金属的富集机制和生物有效性研究[D].南京:南京大学, 2022. Wen Y B. Enrichment mechanism and bioavailability of heavy metals in soil of karst geological high background areas in Guangxi[D]. Nanjing:Nanjing University, 2022. [27] 杨琼,杨忠芳,张起钻,等.中国广西岩溶地质高背景区土壤-水稻系统Cd等重金属生态风险评价[J].中国科学:地球科学, 2021,51:1317-1331. Yang Q, Yang Z F, Zhang Q Z, et al. Ecological risk assessment of heavy metals such as Cd in the soil rice system of karst geological high background areas in Guangxi, China[J]. Chinese Science:Earth Science, 2021,5:1317-1331. [28] Xu Z, Yin M, Yang X, et al.Simulation of vertical migration behaviors of heavy metals in polluted soils from arid regions in northern China under extreme weather[J]. Science of the Total Environment, 2024, 919:170494. [29] Gao T, Ke S, Wang S J, et al.Contrasting Mg isotopic compositions between Fe-Mn nodules and surrounding soils:Accumulation of light Mg isotopes by Mg-depleted clay minerals and Fe oxides[J]. Geochimica et Cosmochimica Acta, 2018,237:205-222. [30] 张良东,杨建军,夏星,等.Eh耦合的稻田土壤镉、砷释放机制[J].环境科学学报, 2020,40(5):1828-1835. Zhang L D, Yang J J, Xia X, et al. Ehcoupled cadmium and arsenic release mechanism in paddy soil[J]. Journal of Environmental Science, 2020,40(5):1828-1835. [31] 中国环境监测总站.中国土壤元素背景值[M].北京:中国环境科学出版社, 1990. China Environmental Monitoring Station. Background values of soil elements in China[M]. Beijing:China Environmental Science Press, 1990. [32] Cheema A I, Liu G, Yousaf B, et al.A comprehensive review of biogeochemical distribution and fractionation of lead isotopes for source tracing in distinct interactive environmental compartments[J]. Science of the Total Environment, 2020,719:135658. [33] Huang Y, Zhang S, Chen Y, et al. Tracing Pb and possible correlated Cd contamination in soils by using lead isotopic compositions[J]. Journal of Hazardous Materials, 2020,385:121528. [34] Liu Y, Xiao T, Zhu J M, et al. Redistribution and isotope fractionation of endogenous Cd in soil profiles with geogenic Cd enrichment[J]. Science of the Total Environment, 2022,852:158447. [35] 方敏雯,王成,熊盈菡,等.基于形态提取与同位素指纹技术研究铅在土壤剖面中的迁移转化--以某铅锌矿周边森林土壤为例[J].地球与环境, 2023,51:235-245. Fang M W, Wang C, Xiong Y H, et al. Study on the migration and transformation of lead in soil profiles based on morphological extraction and isotope fingerprinting techniques:a case study of forest soil around a lead-zinc mine[J]. Earth and Environment, 2023,51:235-245. [36] Esfandbod M, Forghani A, Adhami E, et al. The role of CEC and pH in Cd retention from soils of North of Iran[J]. Soil and Sediment Contamination:An International Journal, 2011,20(8):908-920. [37] 张秋.土地利用方式转变对重金属在土壤中吸附特征和形态分布的影响研究[D].长沙:湖南大学, 2019. Zhang Q. Study on the impact of land use change on the adsorption characteristics and form distribution of heavy metals in soil[D]. Changsha:Hunan University, 2019. [38] Salem MansourA, Bedade D K, AlEthawi L, et al.Assessment of physiochemical properties and concentration of heavy metals in agricultural soils fertilized with chemical fertilizers[J]. Heliyon, 2020,6:e05224. [39] 许子昕.内蒙古典型矿区影响区重金属源解析和垂向运移研究[D].武汉:华中农业大学, 2024. Xu Z X. Source apportionment and vertical transport of heavy metals in the impact area of typical mining areas in Inner Mongolia[D]. Wuhan:Huazhong Agricultural University, 2024. [40] Sterckeman T, Douay F, Baize D, et al.Factors affecting trace element concentrations in soils developed on recent marine deposits from northern France[J]. Applied Geochemistry, 2004,19:89-103. [41] Tack F M G, Vanhaesebroeck T, Verloo M G, et al.Mercury baseline levels in Flemish soils (Belgium)[J]. Environmental Pollution, 2005, 134:173-179. [42] Suda A, Makino T.Functional effects of manganese and iron oxides on the dynamics of trace elements in soils with a special focus on arsenic and cadmium:A review[J]. Geoderma, 2016,270:68-75. [43] 杨琼.广西岩溶区土壤Cd等元素次生富集、生态风险与防控[D].北京:中国地质大学, 2022. Yang Q. Secondary enrichment of Cd and other elements in soil of Karst Areas in Guangxi, ecological risks and prevention and control[D]. Beijing:China University of Geosciences, 2022. [44] Ji W, Lu Y, Zhao C, et al. Mineral composition and environmental importance of Fe-Mn Nodules in soils in Karst Areas of Guangxi, China[J]. Sustainability, 2022,14:12457. [45] 郭超.典型岩溶地质高背景土壤镉生态地球化学研究[D].南京:南京大学, 2022. Guo C. Ecological geochemistry of Cadmium in high background soil of typical Karst Geology[D]. Nanjing:Nanjing University, 2022. [46] Li C, Yang Z, Yu T, Jiang Z, et al. Cadmium accumulation in paddy soils affected by geological weathering and mining:Spatial distribution patterns, bioaccumulation prediction, and safe land usage[J]. Journal of Hazardous Materials, 2023,460:132483. [47] 蒋玉莲.贵州六盘水碳酸盐岩成壤过程中重金属的迁移富集机制[D].北京:中国地质大学, 2022. Jiang Y L. Migration and enrichment mechanism of heavy metals during soil formation of carbonate rocks in Liupanshui, Guizhou[D]. Beijing:China University of Geosciences, 2022. [48] 宣斌,王济,段志斌,等.铅同位素示踪土壤重金属污染源解析研究进展[J].环境科学与技术, 2017,40:17-21. Xuan B, Wang J, Duan Z B, et al. Research progress on lead isotope tracing of soil heavy metal pollution sources[J]. Environmental Science and Technology, 2017,40:17-21. [49] Hu S, Lu Y, Peng L, et al. Coupled kinetics of ferrihydrite transformation and As (V) sequestration under the effect of humic acids:A mechanistic and quantitative study[J]. Environmental Science& Technology, 2018,52(20):11632-11641. [50] 张磊,宋柳霆,郑晓笛,等.溶解有机质与铁氧化物相互作用过程对重金属迁移的影响[J].生态学杂志, 2014,33:2193-2198. Zhang L, Song L T, Zheng X D, et al. The influence of the interaction process between dissolved organic matter and iron oxides on the migration of heavy metals[J]. Ecological Impurities, 2014,33:2193-2198. [51] Quezada-Hinojosa R P, Matera V, Adatte T, et al. Cadmium distribution in soils covering Jurassic oolitic limestone with high Cd contents in the Swiss Jura[J]. Geoderma, 2009,150:287-301. [52] Tessier A P, Campbell P G C, Bisson M X. Sequential extraction procedure for the speciation of particulate trace metals[J]. Analytical Chemistry 1979,51:844. [53] 马宏宏,彭敏,刘飞,等.广西典型碳酸盐岩区农田土壤-作物系统重金属生物有效性及迁移富集特征[J].环境科学, 2020,41(1):449-459. Ma H H, Peng M, Liu F, et al. Biological availability and migration enrichment characteristics of heavy metals in the soil crop system of typical carbonate rock areas in Guangxi[J]. Environmental Science, 2020,41(1):449-459. [54] 杨忠芳.保护国土生态环境安全永续利用资源--解读《广西土地质量地球化学评价报告(2016)》[J].南方国土资源, 2017,2:18-20. Yang Z F.Protecting the national ecological environment security and sustainable utilization of resources-Interpretation of the"Guangxi land quality geochemistry evaluation report (2016)"[J]. Southern Land and Resources, 2017,2:18-20. [55] Bolun Z, Ling L L, Zhan B H, et al. Application of stochastic model to assessment of heavy metal (loid) s source apportionment and bio-availability in rice fields of Karst Area[J]. Science of the Total Environment, 2021,793:148614-148614. [56] Li C, Yang Z F, Tao Y, et al. Study on safe usage of agricultural land in karst and non-karst areas based on soil Cd and prediction of Cd in rice:A case study of Heng County, Guangxi.[J]. Ecotoxicology and Environmental Safety, 2020,208:111505. [57] Grant C N, Dennis H T, Antoine J M R, et al. Agglomerative hierarchical clustering analysis of twenty-six rice samples analysed by instrumental neutron activation analysis and other techniques[J]. Journal of Radioanalytical and Nuclear Chemistry, 2013,297:233-239. [58] Gu Q B, Yang Z F, Yu T, et al.From soil to rice-A typical study of transfer and bioaccumulation of heavy metals in China[J]. Acta Agriculturae Scandinavica and Section B-Soil& Plant Science, 2018, 68:631-642.
