Skip to main content
SpringerLink
Log in

Distribution characteristics of heavy metal(loid)s in aggregates of different size fractions along contaminated paddy soil profile

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Soil aggregates exert a significant influence on the retention and availability of heavy metal(loid)s in soil. In this study, the concentration distribution and chemical forms of heavy metals (Cu, Zn, Cd, Pb, and Hg) and a metalloid (As) in different aggregate-sized fractions (2–0.25, 0.25–0.05, 0.05–0.002, and < 0.002 mm) along the profile (0–1, 1–5, 5–15, and 15–25 cm) of a contaminated paddy field were investigated. The results showed that the values of pH, free Fe oxides (Fed), bulk density, and catalase activity gradually increased, whereas the soil organic matter (SOM), cation exchange capacity (CEC), electrical conductivity (EC), microbial biomass carbon (MBC), and urease activity decreased with depth. Long-term heavy metal pollution might impact the catalase activity but showed no obvious influence on the urease activity. Additionally, there was a notable difference in physicochemical properties among the soil aggregates of various particle sizes. The 2–0.25-mm fraction aggregates contained more organic matter, whereas the highest values of CEC and Fed were observed in the < 0.002-mm fraction. The concentrations of all six heavy metals/metalloid decreased with depth. In different layers, Cu and Cd showed the highest concentrations in the 2–0.25 mm-fraction, followed by the < 0.002-mm fraction, whereas the highest concentrations of Zn, Pb, and As appeared in the < 0.002-mm fraction. No obvious distribution regularity was observed for Hg among the aggregates. All of the metal(loid)s had lower activity in the deeper soil layers, except for Hg. Furthermore, Cu and Cd displayed more stable forms in the < 0.002-mm fraction aggregates.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8

Similar content being viewed by others

References

  • Anderson B, Jenne E (1970) Free-iron and-manganese oxide content of reference clays. Soil Sci 109:163–169

    Article  CAS  Google Scholar 

  • Angers DA, Recous S, Aita C (1997) Fate of carbon and nitrogen in water-stable aggregates during decomposition of 13C15N-labelled wheat straw in situ. Eur J Soil Sci 48:295–300

    Article  Google Scholar 

  • Belic M, Nesic L, Dimitrijevic M, Petrovic S, Ciric V, Pekec S, Vasin J (2012) Impact of reclamation practices on the content and qualitative composition of exchangeable base cations of the solonetz soil. Aust J Crop Sci 6:1471

    Google Scholar 

  • Bradl HB (2004) Adsorption of heavy metal ions on soils and soils constituents. J Colloid Interface Sci 277:1–18

    Article  CAS  Google Scholar 

  • Cao S, Duan X, Zhao X, Ma J, Dong T, Huang N, Sun C, He B, Wei F (2014) Health risks from the exposure of children to As, Se, Pb and other heavy metals near the largest coking plant in China. Sci Total Environ 472:1001–1009

    Article  CAS  Google Scholar 

  • Chen J, He F, Zhang X, Sun X, Zheng J, Zheng J (2014) Heavy metal pollution decreases microbial abundance, diversity and activity within particle-size fractions of a paddy soil. FEMS Microbiol Ecol 87:164–181

    Article  CAS  Google Scholar 

  • Churakov SV, Dähn R (2012) Zinc adsorption on clays inferred from atomistic simulations and EXAFS spectroscopy. Environ Sci Technol 46:5713–5719

    Article  CAS  Google Scholar 

  • Cui H, Ma K, Fan Y, Peng X, Mao J, Zhou D, Zhan Z, Zhou J (2016) Stability and heavy metal distribution of soil aggregates affected by application of apatite, lime, and charcoal. Environ Sci Pollut Res 23:10808–10817

    Article  CAS  Google Scholar 

  • Dahal BM, Fuerhacker M, Mentler A, Karki KB, Shrestha RR, Blum WEH (2008) Arsenic contamination of soils and agricultural plants through irrigation water in Nepal. Environ Pollut 155:157–163

    Article  CAS  Google Scholar 

  • Davidson CM, Duncan AL, Littlejohn D, Ure AM, Garden LM (1998) A critical evaluation of the three-stage BCR sequential extraction procedure to assess the potential mobility and toxicity of heavy metals in industrially-contaminated land. Anal Chim Acta 363:45–55

    Article  CAS  Google Scholar 

  • Fu Q, Gu J, Li Y, Qian X, Sun W, Wang X, Gao H, Zhen L, Lei Y (2015) Analyses of microbial biomass and community diversity in kiwifruit orchard soils of different planting ages. Acta Ecol Sin 35:22–28

    Article  CAS  Google Scholar 

  • GB 15618 (1995) Environmental quality standard for soils. Ministry of Environmental Protection of China. (in Chinese)

  • Gong C, Ma L, Cheng H, Liu Y, Xu D, Li B, Liu F, Ren Y, Zhao C, Yang K, Nie H, Lang C (2014) Characterization of the particle size fraction associated heavy metals in tropical arable soils from Hainan Island, China. J Geochem Explor 139:109–114

    Article  CAS  Google Scholar 

  • Guan S, Zhang D, Zhang Z (1986) Soil enzyme and its research methods. Agricultural, Beijing. (in Chinese)

  • Helling CS, Chesters G, Corey RB (1964) Contribution of organic matter and clay to soil cation-exchange capacity as affected by the pH of the saturating solution. Soil Sci Soc Am J 28:517–520

    Article  CAS  Google Scholar 

  • Hendershot WH, Lalande H, Duquette M (1993) Soil reaction and exchangeable acidity. In: Carter MR (ed) Soil sampling and method of analysis. Lewis publisher, Boca Raton, pp 141–145

  • Huang B, Li Z, Huang J, Guo L, Nie X, Wang Y, Zhang Y, Zeng G (2014) Adsorption characteristics of Cu and Zn onto various size fractions of aggregates from red paddy soil. J Hazard Mater 264:176–183

    Article  CAS  Google Scholar 

  • Huang B, Li Z, Huang J, Chen G, Nie X, Ma W, Yao H, Zhen J, Zeng G (2015) Aging effect on the leaching behavior of heavy metals (Cu, Zn, and Cd) in red paddy soil. Environ Sci Pollut Res 22:11467–11477

    Article  CAS  Google Scholar 

  • Huq SMI, Joardar JC, Parvin S, Correll R, Naidu R (2006) Arsenic contamination in food-chain: transfer of arsenic into food materials through groundwater irrigation. J Health Popul Nutr 24:305–316

    Google Scholar 

  • Khaokaew S, Chaney RL, Landrot G, Ginder-Vogel M, Sparks DL (2011) Speciation and release kinetics of cadmium in an alkaline paddy soil under various flooding periods and draining conditions. Environ Sci Technol 45:4249–4255

    Article  CAS  Google Scholar 

  • Khaokaew S, Landrot G, Chaney RL, Pandya K, Sparks DL (2012) Speciation and release kinetics of zinc in contaminated paddy soils. Environ Sci Technol 46:3957–3963

    Article  CAS  Google Scholar 

  • Kızılkaya R, Aşkın T, Bayraklı B, Sağlam M (2004) Microbiological characteristics of soils contaminated with heavy metals. Eur J Soil Biol 40:95–102

    Article  Google Scholar 

  • Kögel-Knabner I, Amelung W, Cao Z, Fiedler S, Frenzel P, Jahn R, Kalbitz K, Kölbl A, Schloter M (2010) Biogeochemistry of paddy soils. Geoderma 157:1–14

    Article  Google Scholar 

  • Lamb DT, Ming H, Megharaj M, Naidu R (2009) Heavy metal (Cu, Zn, Cd and Pb) partitioning and bioaccessibility in uncontaminated and long-term contaminated soils. J Hazard Mater 171:1150–1158

    Article  CAS  Google Scholar 

  • Lei M, Zhang Y, Khan S, Qin P, Liao B (2010) Pollution, fractionation, and mobility of Pb, Cd, Cu, and Zn in garden and paddy soils from a Pb/Zn mining area. Environ Monit Assess 168:215–222

    Article  CAS  Google Scholar 

  • Li Z, Horikawa Y (1997) Stability behavior of soil colloidal suspensions in relation tosequential reduction of soils: II. Turbidity changes by submergence of paddy soils at different temperatures. Soil Sci Plant Nutr 43:911–919

    Article  Google Scholar 

  • Li Z, Feng X, Li G, Bi X, Sun G, Zhu J, Qin H, Wang J (2011) Mercury and other metal and metalloid soil contamination near a Pb/Zn smelter in east Hunan Province, China. Appl Geochem 26:160–166

    Article  Google Scholar 

  • Li Z, Wu L, Luo Y, Christie P (2014) Dynamics of plant metal uptake and metal changes in whole soil and soil particle fractions during repeated phytoextraction. Plant Soil 374:857–869

    Article  CAS  Google Scholar 

  • Li Z, Huang B, Huang J, Chen G, Zhang C, Nie X, Luo N, Yao H, Ma W, Zeng G (2015) Influence of removal of organic matter and iron and manganese oxides on cadmium adsorption by red paddy soil aggregates. RSC Adv 5:90588–90595

    Article  CAS  Google Scholar 

  • Li Z, Liu C, Dong Y, Chang X, Nie X, Liu L, Xiao H, Lu Y, Zeng G (2017) Response of soil organic carbon and nitrogen stocks to soil erosion and land use types in the loess hilly–gully region of China. Soil Tillage Res 166:1–9

    Article  Google Scholar 

  • Link DD, Walter PJ, Kingston HM (1998) Development and validation of the new EPA microwave-assisted leach method 3051A. Environ Sci Technol 32:3628–3632

    Article  CAS  Google Scholar 

  • Lu C, Zhang J, Jiang H, Yang J, Zhang J, Wang J, Shan H (2010) Assessment of soil contamination with Cd, Pb and Zn and source identification in the area around the Huludao zinc plant. J Hazard Mater 182:743–748

    Article  CAS  Google Scholar 

  • Martín-García JM, Sánchez-Marañón M, Calero J, Aranda V, Delgado G, Delgado R (2016) Iron oxides and rare earth elements in the clay fractions of a soil chronosequence in southern Spain. Eur J Soil Sci 67:749–762

    Article  Google Scholar 

  • Monterroso C, Rodríguez F, Chaves R, Diez J, Becerra-Castro C, Kidd PS, Macías F (2014) Heavy metal distribution in mine-soils and plants growing in a Pb/Zn-mining area in NW Spain. Appl Geochem 44:3–11

    Article  CAS  Google Scholar 

  • Nelson DW, Sommers LE (1982) Total carbon, organic carbon and organic matter. In: Page AL, Miller RH, Keeny DR (eds) Methods of soil analysis. American Society of Agronomy, Wisconsin, pp 539–579

    Google Scholar 

  • Nemati K, Bakar NKA, Abas MR, Sobhanzadeh E (2011) Speciation of heavy metals by modified BCR sequential extraction procedure in different depths of sediments from Sungai Buloh, Selangor, Malaysia. J Hazard Mater 192:402–410

    CAS  Google Scholar 

  • Okkenhaug G, Zhu Y, He J, Li X, Luo L, Mulder J (2012) Antimony (Sb) and arsenic (As) in Sb mining impacted paddy soil from Xikuangshan, China: differences in mechanisms controlling soil sequestration and uptake in rice. Environ Sci Technol 463:155–3162

    Google Scholar 

  • Pan Y, Bonten LTC, Koopmans GF, Song J, Luo Y, Temminghoff EJM, Comans RNJ (2016) Solubility of trace metals in two contaminated paddy soils exposed to alternating flooding and drainage. Geoderma 261:59–69

    Article  CAS  Google Scholar 

  • Parham J, Deng S, Raun W, Johnson G (2002) Long-term cattle manure application in soil. Biol Fertil Soils 35:328–337

    Article  CAS  Google Scholar 

  • Pen-Mouratov S, Shukurov N, Steinberger Y (2008) Influence of industrial heavy metal pollution on soil free-living nematode population. Environ Pollut 152:172–183

    Article  CAS  Google Scholar 

  • Qian J, Shan XQ, Wang ZJ, Tu Q (1996) Distribution and plant availability of heavy metals in different particle-size fractions of soil. Sci Total Environ 187:131–141

    Article  CAS  Google Scholar 

  • Quenea K, Lamy I, Winterton P, Bermond A, Dumat C (2009) Interactions between metals and soil organic matter in various particle size fractions of soil contaminated with waste water. Geoderma 149:217–223

    Article  CAS  Google Scholar 

  • Rodríguez L, Ruiz E, Alonso-Azcárate J, Rincón J (2009) Heavy metal distribution and chemical speciation in tailings and soils around a Pb–Zn mine in Spain. J Environ Manag 90:1106–1116

    Article  Google Scholar 

  • Schmidt MWI, Rumpel C, Kögel-Knabner I (1999) Evaluation of an ultrasonic dispersion procedure to isolate primary organomineral complexes from soils. Eur J Soil Sci 50:87–94

    Article  Google Scholar 

  • Seyfferth AL, McCurdy S, Schaefer MV, Fendorf S (2014) Arsenic concentrations in paddy soil and rice and health implications for major rice-growing regions of Cambodia. Environ Sci Technol 48:4699–4706

    Article  CAS  Google Scholar 

  • Simmons RW, Pongsakul P, Saiyasitpanich D, Klinphoklap S (2005) Elevated levels of cadmium and zinc in paddy soils and elevated levels of cadmium in rice grain downstream of a zinc mineralized area in Thailand: implications for public health. Environ Geochem Health 27:501–511

    Article  CAS  Google Scholar 

  • Six J, Paustian K, Elliott ET (2000) Soil structure and organic matter. I. Distribution of aggregate-size classes and aggregate-associated carbon. Soil Sci Soc Am J 64:681–689

    Article  CAS  Google Scholar 

  • Su C, Jiang L, Zhang W (2014) A review on heavy metal contamination in the soil worldwide: situation, impact and remediation techniques. Environ Skep Crit 3:24–38

    Google Scholar 

  • The Ministry of Environmental Protection (2014) The Ministry of Land and Resources report on the national soil contamination survey http://www.mep.gov.cn/gkml/hbb/qt/201404/t20140417_270670.htm. Accessed 27 Aug 2014

  • Udawatta RP, Kremer RJ, Adamson BW, Anderson SH (2008) Variations in soil aggregate stability and enzyme activities in a temperate agroforestry practice. Appl Soil Ecol 39:153–160

    Article  Google Scholar 

  • Vance ED, Brookes PC, Jenkinson DS (1987) An extraction method for measuring soil microbial biomass C. Soil Biol Biochem 19:703–707

    Article  CAS  Google Scholar 

  • Wenzel WW, Kirchbaumer N, Prohaska T, Stingeder G, Lombi E, Adriano DC (2001) Arsenic fractionation in soils using an improved sequential extraction procedure. Anal Chim Acta 436:309–323

    Article  CAS  Google Scholar 

  • Williams PN, Lei M, Sun G, Huang Q, Lu Y, Deacon C, Meharg AA, Zhu Y (2009) Occurrence and partitioning of cadmium, arsenic and lead in mine impacted paddy rice: Hunan, China. Environ Sci Technol 43:637–642

    Article  CAS  Google Scholar 

  • Wu H, Jiang D, Cai P, Rong X, Dai K, Liang W, Huang Q (2012) Adsorption of Pseudomonas putida on soil particle size fractions: effects of solution chemistry and organic matter. J Soils Sediments 12:143–149

    Article  CAS  Google Scholar 

  • Yang S, Zhou D, Yu H, Wei R, Pan B (2013) Distribution and speciation of metals (Cu, Zn, Cd, and Pb) in agricultural and non-agricultural soils near a stream upriver from the Pearl River, China. Environ Pollut 177:64–70

    Article  CAS  Google Scholar 

  • Zeng F, Ali S, Zhang H, Ouyang Y, Qiu B, Wu F, Zhang G (2011) The influence of pH and organic matter content in paddy soil on heavy metal availability and their uptake by rice plants. Environ Pollut 159:84–91

    Article  CAS  Google Scholar 

  • Zhang L, Li L, Pan G, Cui L, Li H, Wu X, Shao J (2009) Effect of heavy metals pollution on paddy soil aggregates composition and heavy metals distribution. Chin J Appl Ecol 20:2806–2812 (in Chinese)

    CAS  Google Scholar 

  • Zhang S, Li Q, Zhang X, Wei K, Chen L, Liang W (2012) Effects of conservation tillage on soil aggregation and aggregate binding agents in black soil of Northeast China. Soil Tillage Res 124:196–202

    Article  Google Scholar 

  • Zhang H, Luo Y, Makino T, Wu L, Nanzyo M (2013) The heavy metal partition in size-fractions of the fine particles in agricultural soils contaminated by waste water and smelter dust. J Hazard Mater 248:303–312

    Article  Google Scholar 

  • Zhao K, Liu X, Xu J, Selim HM (2010) Heavy metal contaminations in a soil–rice system: identification of spatial dependence in relation to soil properties of paddy fields. J Hazard Mater 181:778–787

    Article  CAS  Google Scholar 

  • Zhao F, Ma Y, Zhu Y, Tang Z, McGrath SP (2014) Soil contamination in China: current status and mitigation strategies. Environ Sci Technol 49:750–759

    Article  Google Scholar 

  • Zheng X, Xia B, Lin X (2010) Variation of total organic carbon and particulate and organic carbon in paddy soils contaminated by heavy metals. China Environ Sci 30:369–373 (in Chinese)

    CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by the GDAS’ Special Project of Science and Technology Development (2017GDASCX-0830), the Natural Science Foundation of China (Nos. 41701320, 41501298 and 51521006), the High-level Leading Talent Introduction Program (2060599), the SPICC Program (The Scientific Platform and Innovation Capability Construction Program of GDAS, 2016GDASPT-0105 and 0304), the Construction of Innovative Talents for Pollution Control and Management of Heavy Metals in Farmland (2016B070701015), and Key Research Items in Science and Technology Program from China Hunan Provincial Science and Technology Department (No. 2015SK2004). We would like to thank Ninglin Luo, Qiu Zhang, Mei Huang, and Xiuqing Zhai of Hunan University for the sampling and laboratory analysis.

Author information

Authors and Affiliations

  1. Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management, Guangdong Institute of Eco-environmental Science & Technology, Guangzhou, 510650, China

    Bin Huang, Dingqiang Li & Zaijian Yuan

  2. College of Environmental Science and Engineering, Hunan University, Changsha, 410082, China

    Zhongwu Li

  3. Key Laboratory of Environment Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, 410082, China

    Zhongwu Li

  4. Ministry of Environment Protection, South China Institute of Environmental Science, Guangzhou, 510655, China

    Zhiliang Chen

  5. Department of Soil and Water Conservation, Yangtze River Scientific Research Institute, Wuhan, 430010, China

    Jinquan Huang

Authors
  1. Bin Huang
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Zhongwu Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Dingqiang Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Zaijian Yuan
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Zhiliang Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Jinquan Huang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Zhongwu Li or Dingqiang Li.

Ethics declarations

The manuscript has not been submitted to more than one journal for simultaneous consideration and has not been published previously (partly or in full).

A single study is not split up into several parts to increase the quantity of submissions and submitted to various journals or to one journal over time.

No data have been fabricated or manipulated (including images) to support the conclusions.

No data, text, or theories by others are presented as if they were our own. Proper acknowledgements have been given, quotation marks are used for verbatim copying of material, and permissions are secured for material that is copyrighted.

Consent to submit has been received explicitly from all co-authors.

Authors whose names appear on the submission have contributed sufficiently to the scientific work and therefore share collective responsibility and accountability for the results.

Conflict of interest

The authors declare that they have no conflict of interest.

Additional information

Responsible editor: Zhihong Xu

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Huang, B., Li, Z., Li, D. et al. Distribution characteristics of heavy metal(loid)s in aggregates of different size fractions along contaminated paddy soil profile. Environ Sci Pollut Res 24, 23939–23952 (2017). https://doi.org/10.1007/s11356-017-0012-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-017-0012-4

Keywords

Search

Navigation