Abstract
In this work, a new resin gel incorporated with layered double hydroxide nanoparticles modified with diethylenetriaminepentaacetic acid is developed for application in diffusive gradients in thin-film devices (abbreviated as LDHs DGT) to monitor eight anions and cations (such as Fe, Mn, Co, Ni, Cu, Cd, Pb, and As) in natural waters and soils. The accumulated anions and cations were quantitatively recovered by one-step elution using 0.5 mol·L−1 HNO3 with an optimized elution time of 30 min. The performance of the LDHs DGT was independent of solution pH (5–8) and ionic strengths (5–100 mmol·L−1). The capacities of the LDHs DGT for Mn(II), Fe(II), Co(II), Ni(II), Cu(II), As(V), Cd(II), and Pb(II) individually are determined to be 202.9, 363.6, 246.9, 88.8, 99.5, 75.3, 159.8, and 671.7 μg·cm−2. During the field deployments in a nature river, LDHs DGT measured concentrations of cations and anions were almost like those measured by the traditional sampling method (except Fe(II), Cd(II), and Co(II)). In addition, bioavailable Cd measured by LDHs DGT correlated well with Cd in rice grains (R2 = 0.55), indicating that LDHs DGT is a reliable tool for assessing the risk of Cd.
Similar content being viewed by others
Data availability
Not applicable.
References
Bennett WW, Teasdale PR, Panther JG, Welsh DT, Jolley DF (2010) New Diffusive gradients in a thin film technique for measuring inorganic arsenic and selenium(IV) using a titanium dioxide based adsorbent. Anal Chem 82:7401–7407
Buchberger W, Mulleder S (1995) Determination of chelating-agents and metal-chelates by capillary zone electrophoresis. Mikrochim Acta 119:103–111
Chen R, Gao T, Cheng N, Ding G, Wang Q, Shi R, Hu G, Cai X (2021): Application of DGT/DIFS to assess bioavailable Cd to maize and its release in agricultural soils. J Hazard Mater 411:124837
Cornu J-Y, Denaix L, Lacoste J, Sappin-Didier V, Nguyen C, Schneider A (2016) Impact of temperature on the dynamics of organic matter and on the soil-to-plant transfer of Cd, Zn and Pb in a contaminated agricultural soil. Environ Sci Pollut Res 23:2997–3007
Davison W, Zhang H (2012) Progress in understanding the use of diffusive gradients in thin films (DGT) - back to basics. Environ Chem 9:1–13
Ding S, Sun Q, Xu D, Jia F, He X, Zhang C (2012) High-resolution simultaneous measurements of dissolved reactive phosphorus and dissolved sulfide: the first observation of their simultaneous release in sediments. Environ Sci Technol 46:8297–8304
Ding S, Xu D, Wang Y, Wang Y, Li Y, Gong M, Zhang C (2016) Simultaneous measurements of eight oxyanions using high-capacity diffusive gradients in thin films (Zr-Oxide DGT) with a high-efficiency elution procedure. Environ Sci Technol 50:7572–7580
Drozdzak J, Leermakers M, Gao Y, Phrommavanh V, Descostes M (2016) Novel speciation method based on diffusive gradients in thin films for in situ measurement of uranium in the vicinity of the former uranium mining sites. Environ Pollut 214:114–123
Du HH, PeacocK CL, Chen WL, Huang QY (2018) Binding of Cd by ferrihydrite organo-mineral composites: implications for Cd mobility and fate in natural and contaminated environments. Chemosphere 207:404–412
Gao X, Chen C-TA (2012) Heavy metal pollution status in surface sediments of the coastal Bohai Bay. Water Res 46:1901–1911
Garmo OA, Davison W, Zhang H (2008) Interactions of trace metals with hydrogels and filter membranes used in DET and DGT techniques. Environ Sci Technol 42:5682–5687
Gu S, Kang X, Wang L, Lichtfouse E, Wang C (2019) Clay mineral adsorbents for heavy metal removal from wastewater: a review. Environ Chem Lett 17:629–654
Guan DX, Williams PN, Luo J, Zheng JL, Xu HC, Cai C, Ma LQ (2015) Novel precipitated zirconia-based DGT technique for high-resolution imaging of oxyanions in waters and sediments. Environ Sci Technol 49:3653–3661
Guan DX, Williams PN, Xu HC, Li G, Luo J, Ma LQ (2016) High-resolution measurement and mapping of tungstate in waters, soils and sediments using the low-disturbance DGT sampling technique. J Hazard Mater 316:69–76
Guan DX, Li YQ, Yu NY, Yu GH, Wei S, Zhang H, Davison W, Cui XY, Ma LQ, Luo J (2018) In situ measurement of perfluoroalkyl substances in aquatic systems using diffusive gradients in thin-films technique. Water Res 144:162–171
Guan DX, He SX, Li G, Teng HH, Ma LAQ (2022) Application of diffusive gradients in thin-films technique for speciation, bioavailability, modeling and mapping of nutrients and contaminants in soils. Crit Rev Environ Sci Technol 52:3035–3079
Jiang X, Zhang M, Yan B, Hu J, Chen J, Guan Y (2019) Roles of Mg-Al layered double hydroxides and solution chemistry on P transport in soil. Chem Eng J 373:1111–1119
Kang D, Yu X, Tong S, Ge M, Zuo J, Cao C, Song W (2013) Performance and mechanism of Mg/Fe layered double hydroxides for fluoride and arsenate removal from aqueous solution. Chem Eng J 228:731–740
Kreuzeder A, Santner J, Prohaska T, Wenzel WW (2013) Gel for simultaneous chemical imaging of anionic and cationic solutes using diffusive gradients in thin films. Anal Chem 85:12028–12036
Li C-M, Lei C-X, Liang Y-T, Chen C-Q, Sun B (2016) As contamination alters rhizosphere microbial community composition with soil type dependency during the rice growing season. Paddy Water Environ 15:581–592
Li K, Liu Z, Shi X, Wei T-j, Ma LQ, Luo J (2020): Novel in situ method based on diffusive gradients in thin-films with lanthanum oxide nanoparticles for measuring As, Sb, and V and in waters. J Hazard Mater 383:121196
Liang X, Hou W, Xu Y, Sun G, Wang L, Sun Y, Qin X (2010) Sorption of lead ion by layered double hydroxide intercalated with diethylenetriaminepentaacetic acid. Colloids Surf A: Physicochem Eng Asp 366:50–57
Liang L, Yang W, Guan X, Li J, Xu Z, Wu J, Huang Y, Zhang X (2013) Kinetics and mechanisms of pH-dependent selenite removal by zero valent iron. Water Res 47:5846–5855
Liang X, Zang Y, Xu Y, Tan X, Hou W, Wang L, Sun Y (2013) Sorption of metal cations on layered double hydroxides. Colloids Surf A: Physicochem Eng Asp 433:122–131
Liu HM, Zhao XJ, Zhu YQ, Yan H (2020) DFT study on MgAl-layered double hydroxides with different interlayer anions: structure, anion exchange, host-guest interaction and basic sites. Phys Chem Chem Phys 22:2521–2529
Luo J, Zhang H, Santner J, Davison W (2010) Performance characteristics of diffusive gradients in thin films equipped with a binding gel layer containing precipitated ferrihydrite for measuring arsenic(V), selenium(VI), vanadium(V), and antimony(V). Anal Chem 82:8903–8909
Ma Q, Zhao W, Guan DX, Teng HH, Ji J, Ma LQ (2020) Comparing CaCl2, EDTA and DGT methods to predict Cd and Ni accumulation in rice grains from contaminated soils. Environ Pollut 260:114042
Mason S, Hamon R, Nolan A, Zhang H, Davison W (2005) Performance of a mixed binding layer for measuring anions and cations in a single assay using the diffusive gradients in thin films technique. Anal Chem 77:6339–6346
Maziarz P, Matusik J, Straczek T, Kapusta C, Woch WM, Tokarz W, Radziszewska A, Leiviska T (2019) Highly effective magnet-responsive LDH-Fe oxide composite adsorbents for As(V) removal. Chem Eng J 362:207–216
Menegario AA, Tonello PS, Durrant SF (2010) Use of Saccharomyces cerevisiae immobilized in agarose gel as a binding agent for diffusive gradients in thin films. Anal Chim Acta 683:107–112
Osterlund H, Chlot S, Faarinen M, Widerlund A, Rodushkin I, Ingri J, Baxter DC (2010) Simultaneous measurements of As, Mo, Sb, V and W using a ferrihydrite diffusive gradients in thin films (DGT) device. Anal Chim Acta 682:59–65
Paller MH, Harmon SM, Knox AS, Kuhne WW, Halverson NV (2019): Assessing effects of dissolved organic carbon and water hardness on metal toxicity to Ceriodaphnia dubia using diffusive gradients in thin films (DGT). Sci Total Environ 697:134107
Pan Y, Guan D-X, Zhao D, Luo J, Zhang H, Davison W, Ma LQ (2015) Novel speciation method based on diffusive gradients in thin-films for in situ measurement of Cr-VI in aquatic systems. Environ Sci Technol 49:14267–14273
Pan F, Liu H, Guo Z, Cai Y, Fu Y, Wu J, Wang B, Gao A (2019): Metal/metalloid and phosphorus characteristics in porewater associated with manganese geochemistry: a case study in the Jiulong River Estuary, China. Environ Pollut 255:113134
Panther JG, Stewart RR, Teasdale PR, Bennett WW, Welsh DT, Zhao H (2013) Titanium dioxide-based DGT for measuring dissolved As(V), V(V), Sb(V), Mo(VI) and W(VI) in water. Talanta 105:80–86
Panther JG, Bennett WW, Welsh DT, Teasdale PR (2014) Simultaneous measurement of trace metal and oxyanion concentrations in water using diffusive gradients in thin films with a Chelex-Metsorb mixed binding layer. Anal Chem 86:427–434
Price HL, Teasdale PR, Jolley DF (2013) An evaluation of ferrihydrite- and Metsorb (TM)-DGT techniques for measuring oxyanion species (As, Se, V, P): effective capacity, competition and diffusion coefficients. Anal Chim Acta 803:56–65
Smolders E, Wagner S, Prohaska T, Irrgeher J, Santner J (2020) Sub-millimeter distribution of labile trace element fluxes in the rhizosphere explains differential effects of soil liming on cadmium and zinc uptake in maize. Sci Total Environ 738:140311
Stockdale A, Davison W, Zhang H (2008) High-resolution two-dimensional quantitative analysis of phosphorus, vanadium and arsenic, and qualitative analysis of sulfide, in a freshwater sediment. Environ Chem 5:143–149
Sun Q, Ding S, Wang Y, Xu L, Wang D, Chen J, Zhang C (2016) In-situ characterization and assessment of arsenic mobility in lake sediments. Environ Pollut 214:314–323
Tan F, Wang Y, Wang Y, Ren S, Cui Y, Xu D (2020) Ceria oxide nanoparticle-based diffusive gradients in thin films for in situ measurement of dissolved reactive phosphorus in waters and sewage sludge. Environ Sci Pollut Res 27:11138–11146
Trang H, Zhang H, Noller B (2012) Evaluation and application of the diffusive gradients in thin films technique using a mixed-binding gel layer for measuring inorganic arsenic and metals in mining impacted water and soil. Anal Chem 84:9988–9995
van Leeuwen HP (2016) Revisited: DGT speciation analysis of metal-humic acid complexes. Environ Chem 13:84–88
Wang Y, Ding S, Gong M, Xu S, Xu W, Zhang C (2016) Diffusion characteristics of agarose hydrogel used in diffusive gradients in thin films for measurements of cations and anions. Anal Chim Acta 945:47–56
Wang Y, Ding S, Shi L, Gong M, Xu S, Zhang C (2017) Simultaneous measurements of cations and anions using diffusive gradients in thin films with a ZrO-Chelex mixed binding layer. Anal Chim Acta 972:1–11
Wang Y, Ding S, Ren M, Li C, Xu S, Sun Q, Xu L (2019) Enhanced DGT capability for measurements of multiple types of analytes using synergistic effects among different binding agents. Sci Total Environ 657:446–456
Williams PN, Zhang H, Davison W, Meharg AA, Hossain M, Norton GJ, Brammer H, Islam MR (2011) Organic matter-solid phase interactions are critical for predicting arsenic release and plant uptake in bangladesh paddy soils. Environ Sci Technol 45:6080–6087
Williams PN, Zhang H, Davison W, Zhao S, Lu Y, Dong F, Zhang L, Pan Q (2012) Evaluation of in situ DGT measurements for predicting the concentration of Cd in chinese field-cultivated rice: impact of soil Cd: Zn ratios. Environ Sci Technol 46:8009–8016
Xu D, Chen Y, Ding S, Sun Q, Wang Y, Zhang C (2013) Diffusive gradients in thin films technique equipped with a mixed binding gel for simultaneous measurements of dissolved reactive phosphorus and dissolved iron. Environ Sci Technol 47:10477–10484
Yin DX, Fang W, Guan DX, Williams PN, Moreno-Jimenez E, Gao Y, Zhao FJ, Ma LQ, Zhang H, Luo J (2020): Localized intensification of arsenic release within the emergent rice rhizosphere. Environ Sci Technol 54:3138–3147
Zhang H, Davison W (1995) Performance-characteristics of diffusion gradients in thin-films for the in-situ measurement of trace-metals in aqueous-solution. Anal Chem 67:3391–3400
Zhang H, Davison W, Knight B, McGrath S (1998) In situ measurements of solution concentrations and fluxes of trace metals in soils using DGT. Environ Sci Technol 32:704–710
Zhang H, Zhao FJ, Sun B, Davison W, McGrath SP (2001) A new method to measure effective soil solution concentration predicts copper availability to plants. Environ Sci Technol 35:2602–2607
Zhou Z, Muehe EM, Tomaszewski EJ, Lezama-Pacheco J, Kappler A, Byrne JM (2020) Effect of natural organic matter on the fate of cadmium during microbial ferrihydrite reduction. Environ Sci Technol 54:9445–9453
Funding
This work was supported by the Agricultural Science and Technology Achievements Transformation and Extension Project of Tianjin (201901250).
Author information
Authors and Affiliations
Contributions
All authors contributed to the study conception and design. Material preparation and data collection were performed by Zhen Wang and Qian E. Data analysis and curation were performed Zhen Wang, Qian E, Chuangchuang Zhang, Jiang Liu, Xuefeng Liang, and Yujie Zhao. The first draft of the manuscript was written by Zhen Wang and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.
Corresponding author
Ethics declarations
Ethics approval
Not applicable.
Consent to participate
Not applicable.
Consent for publication
Not applicable.
Conflict of interest
The authors declare no competing interests.
Additional information
Responsible Editor: Luke Mosley
Publisher's note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Wang, Z., Er, Q., Zhang, C. et al. A new DGT technique based on nano-sized Mg2Al layered double hydroxides with DTPA for sampling of eight anionic and cationic metals. Environ Sci Pollut Res 30, 37679–37690 (2023). https://doi.org/10.1007/s11356-022-24905-6
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-022-24905-6