Abstract
Recently, a sponge-like material called carbon nanotube sponges (CNT sponges) has drawn considerable attention because it can remove large-area oil, nanoparticles, and organic dyes from water. In this paper, the feasibility of CNT sponges as a novel solid-phase extraction (SPE) adsorbent for the enrichment and determination of heavy metal ions (Co2+, Cu2+, and Hg2+) was investigated for the first time. Sodium diethyldithiocarbamate (DDTC) was used as the chelating agent and high performance liquid chromatography (HPLC) for the final analysis. Important factors which may influence extraction efficiency of SPE were optimized, such as the kind and volume of eluent, volume of DDTC, sample pH, flow rate, etc. Under the optimized conditions, wide range of linearity (0.5–400 μg L−1), low limits of detection (0.089~0.690 μg L−1; 0.018~0.138 μg), and good repeatability (1.27~3.60 %, n = 5) were obtained. The developed method was applied for the analysis of the three metal ions in real water samples, and satisfactory results were achieved. All of these findings demonstrated that CNT sponges will be a good choice for the enrichment and determination of target ions at trace levels in the future.
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Crini G. Recent developments in polysaccharide-based materials used as adsorbents in wastewater treatment. Prog Polym Sci. 2005;30:38–70.
Coen N, Mothersill C, Kadhim M, Wright EG. Heavy metals of relevance to human health induce genomic instability. J Pathol. 2001;195:293–9.
Wang Y, Ke X, Zhou X, Li J, Ma J. Graphene for separation and preconcentration of trace amounts of cobalt in water samples prior to flame atomic absorption spectrometry. J Saudi Chem Soc. 2015 ;19:129–136.
Xu H, Zeng L, Xing S, Shi G, Xian Y, Jin L. Microwave-radiated synthesis of gold nanoparticles/carbon nanotubes composites and its application to voltammetric detection of trace mercury(II). Electrochem Commun. 2008;10:1839–43.
Abas MRB, TakruniI IA, Abdullah Z, Tahir NM. On-line preconcentration and determination of trace metals using a flow injection system coupled to ion chromatography. Talanta. 2002;58:883–90.
El-Shahawi MS, Al-Saidi HM. Dispersive liquid-liquid microextraction for chemical speciation and determination of ultra-trace concentrations of metal ions. Trends Anal Chem. 2013;44:12–24.
Li W, Zhao H, Teasdale PR, John R, Zhang S. Application of a cellulose phosphate ion exchange membrane as a binding phase in the diffusive gradients in thin films technique for measurement of trace metals. Anal Chim Acta. 2002;464:331–9.
Feist B, Mikula B. Preconcentration of heavy metals on activated carbon and their determination in fruits by inductively coupled plasma optical emission spectrometry. Food Chem. 2014;147:302–6.
Chen D, Hu B, Huang C. Chitosan modified ordered mesoporous silica as micro-column packing materials for on-line flow injection-inductively coupled plasma optical emission spectrometry determination of trace heavy metals in environmental water samples. Talanta. 2009;78:491–7.
Bulut VN, Duran C, Gundogdu A, Soylak M, Yildirim N, Elci L. A new approach to separation and pre-concentration of some trace metals with co-precipitation method using a triazole. Talanta. 2008;76:469–74.
Tuzen M, Soylak M. Multiwalled carbon nanotubes for speciation of chromium in environmental samples. J Hazard Mater. 2007;147:219–25.
Fan J, Wu C, Wei Y, Peng C, Peng P. Preparation of xylenol orange functionalized silica gel as a selective solid phase extractor and its application for preconcentration-separation of mercury from waters. J Hazard Mater. 2007;145:323–30.
Vieira EG, Soares IV, Dias Filho NL, da Silva NC, Garcia EF, Bastos AC, et al. Preconcentration and determination of metal ions from fuel ethanol with a new 2,2-dipyridylamine bonded silica. J Colloid Interf Sci. 2013;391:116–24.
Hu B, He M, Chen B. Nanometer-sized materials for solid-phase extraction of trace elements. Anal Bioanal Chem. 2015;407:2685–710.
Peng H, Zhang N, He M, Chen B, Hu B. Simultaneous speciation analysis of inorganic arsenic, chromium and selenium in environmental waters by 3-(2-aminoethylamino) propyltrimethoxysilane modified multi-wall carbon nanotubes packed microcolumn solid phase extraction and ICP-MS. Talanta. 2015;131:266–72.
Gustavo Rocha de C, Ilton Luiz de A, Paulo dos Santos R. Synthesis, characterization and determination of the metal ions adsorption capacity of cellulose modified with p-aminobenzoic groups. Mater Res. 2004;7:329–34.
Mauter MS, Elimelech M. Environmental applications of carbon-based nanomaterials. Environ Sci Technol. 2008;42:5843–5859.
Pan B, Xing B. Adsorption mechanisms of organic chemicals on carbon nanotubes. Environ Sci Technol. 2008;42:9005–13.
Gui X, Wei J, Wang K, Cao A, Zhu H, Jia Y, et al. Carbon nanotube sponges. Adv Mater. 2010;22:617–21.
Li H, Gui X, Zhang L, Wang S, Ji C, Wei J, et al. Carbon nanotube sponge filters for trapping nanoparticles and dye molecules from water. Chem Commun. 2010;46:7966–8.
Gui X, Li H, Wang K, Wei J, Jia Y, Li Z, et al. Recyclable carbon nanotube sponges for oil absorption. Acta Mater. 2011;59:4798–804.
Chai X, Chang X, Hu Z, He Q, Tu Z, Li Z. Solid phase extraction of trace Hg(II) on silica gel modified with 2-(2-oxoethyl)hydrazine carbothioamide and determination by ICP-AES. Talanta. 2010;82:1791–6.
Jiao F, Gao H. On-site solid-phase extraction and application to in situ preconcentration of heavy metals in surface water. Environ Monit Assess. 2013;185:39–44.
Bakircioglu D, Topraksever N, Kurtulus YB. Determination of zinc in edible oils by flow injection FAAS after extraction induced by emulsion breaking procedure. Food Chem. 2014;151:219–24.
Long XB, Miró M, Jensen R, Hansen EH. Highly selective micro-sequential injection lab-on-valve (μSI-LOV) method for the determination of ultra-trace concentrations of nickel in saline matrices using detection by electrothermal atomic absorption spectrometry. Anal Bioanal Chem. 2006;386:739–48.
Kagaya S, Takata D, Yoshimori T, Kanbara T, Tohda K. A sensitive and selective method for determination of gold(III) based on electrothermal atomic absorption spectrometry in combination with dispersive liquid–liquid microextraction using dicyclohexylamine. Talanta. 2010;80:1364–70.
Zhang N, Peng H, Wang S, Hu B. Fast and selective magnetic solid phase extraction of trace Cd, Mn and Pb in environmental and biological samples and their determination by ICP-MS. Microchim Acta. 2011;175:121–8.
Aliaga-Campuzano MP, Bernal JP, Briceño-Prieto SB, Pérez-Arvizua O, Lounejeva E. Direct analysis of lanthanides by ICP-MS in calcium-rich water samples using a modular high-efficiency sample introduction system–membrane desolvator. J Anal Atom Spectrom. 2013;28:1102–9.
Sarzanini C, Bruzzoniti MC. Metal species determination by ion chromatography. Trends Anal Chem. 2001;20:304–10.
Martín-Esteban A, Garcinuno R, Angelino S, Fernandez P, Camara C. Determination of trace metals in waters and compost by on-line precipitation coupled to flame atomic absorption spectrophotometry or ion chromatography. Talanta. 1999;48:959–66.
Wei Z, Wong J, Chen D. Speciation of heavy metal binding non-protein thiols in Agropyron elongatum by size-exclusion HPLC–ICP-MS. Microchem J. 2003;74:207–13.
Gregori I, Quiroz W, Pinochet H, Pannier F, Potin-Gautier M. Simultaneous speciation analysis of Sb(III), Sb(V) and (CH3)3SbCl2 by high performance liquid chromatography-hydride generation-atomic fluorescence spectrometry detection (HPLC-HG-AFS): application to antimony speciation in sea water. J Chromatogr A. 2005;1091:94–101.
Tófalvi R, Horváth K, Hajós P. High performance ion chromatography of transition metal chelate complexes and aminopolycarboxylate ligands. J Chromatogr A. 2013;1272:6–32.
Zhou Q, Xiao J, Wang W. Using multi-walled carbon nanotubes as solid phase extraction adsorbents to determine dichlorodiphenyltrichloroethane and its metabolites at trace level in water samples by high performance liquid chromatography with UV detection. J Chromatogr A. 2006;1125:152–258.
Peng X, Pang J, Deng A, Liang W, Liang Y, Wen Q. Determination of the trace residues of four organochlorine pesticides in agricultural products by high performance liquid chromatography with modified multi-walled carbon nanotubes as solid phase extraction adsorbent. Chin J Chromatogr. 2012;30:966–70 (in Chinese).
Wang W, Huang Y, Shu W, Cao J. Multiwalled carbon nanotubes as adsorbents of solid-phase extraction for determination of polycyclic aromatic hydrocarbons in environmental waters coupled with high-performance liquid chromatography. J Chromatogr A. 2007;1173:27–36.
Kanbayashi M, Hoshino H, Yotsuyanagi T. Highly selective determination of trace amounts of copper(II), nickel(II) and vanadium(V) ions with tetradentate schiff-base ligands by reversed-phase high performance liquid chromatography and spectrophotometric detection. J Chromatogr. 1987;386:191–7.
Chand V, Prasad S. ICP-OES assessment of heavy metal contamination in tropical marine sediments: a comparative study of two digestion techniques. Microchem J. 2013;111:53–61.
Zhao R, Wang X, Yuan J, Lin J. Investigation of feasibility of bamboo charcoal as solid-phase extraction adsorbent for the enrichment and determination of four phthalate esters in environmental water samples. J Chromatogr A. 2008;1183:15–20.
Zhou Q, Xing A, Zhao K. Simultaneous determination of nickel, cobalt and mercury ions in water samples by solid phase extraction using multiwalled carbon nanotubes as adsorbent after chelating with sodiumdiethyldithiocarbamate prior to high performance liquid chromatography. J Chromatogr A. 2014;1360:76–81.
Zhou Q, Wu W, Xie G. Solid phase extraction with silicon dioxide microsphere adsorbents in combination with gas chromatographyelectron capture detection for the determination of DDT and its metabolites in water samples. J Environ Sci Health. 2013;48:191–7.
Sitki B, Erdal K, Turker AR. Separation/preconcentration of Zn(II), Cu(II), and Cd(II) by Saccharomyces carlsbergensis immobilized on silica gel 60 in various samples. Sep Sci Technol. 2006;41:3449–65.
Hüseyin B, Aydan E, Latif E. Determination of lead, iron, manganese and zinc in sea water samples by atomic absorption spectrometry after preconcentration with chromosorb 105. Anal Chem. 2006;1:42–54.
Asghari A, Ghazaghi M, Rajabi M, Behzad M, Ghaedi M. Ionic liquid-based dispersive liquid–liquid microextraction combined with high performance liquid chromatography–UV detection for the simultaneous pre-concentration and determination of Ni, Co, Cu and Zn in water samples. J Serb Chem Soc. 2014;79:63–76.
Liu B, Zhang H, Ma Y. Determination of several heavy metal ions by HPLC coupled with sugar-induced phase-separation. Guangzhou Chem Ind Technol. 2011;6:106–12.
Supalax S, Wijitra A, Yanawath S, Tipwan K, Archava S, Richard L. Use of 1-(2-pyridylazo)-2-naphthol as the post column reagent for ion exchange chromatography of heavy metals in environmental samples. Microchem J. 2011;99:152–8.
Huang K, Jiang S. Determination of trace levels of metal ions in water samples by inductively coupled plasma mass spectrometry after on-line preconcentration on SO3-oxine CM-cellulose. Fresenius J Anal Chem. 1993;347:238–42.
Acknowledgments
This study was supported by the National Natural Science Foundation of China (21477068, 21277108, and 21277084), Natural Science Foundation of Shandong Province (ZR2015YL003), Key Research and Development Program of Shandong Province (2015GSF117011), and Research Encouragement Foundation of Excellent Midlife-Youth Scientists of Shandong Province (BS2012HZ012).
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Wang, L., Zhou, JB., Wang, X. et al. Simultaneous determination of copper, cobalt, and mercury ions in water samples by solid-phase extraction using carbon nanotube sponges as adsorbent after chelating with sodium diethyldithiocarbamate prior to high performance liquid chromatography. Anal Bioanal Chem 408, 4445–4453 (2016). https://doi.org/10.1007/s00216-016-9542-8
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DOI: https://doi.org/10.1007/s00216-016-9542-8