Abstract
Presence of carcinogenic chromium, i.e., Cr(VI), in different industrial effluents necessitates design and development of effective abatement technologies. Nanosorbent consisting of iron oxide nanoparticles functionalized with soil-derived humic acid was employed for removal of Cr(VI). The point of zero charge for both humic acid and nanoparticles as estimated from pH shift experiments was between pH 8 and 9. Adsorption isotherm from batch experiments at neutral pH followed Langmuir model with projected maximum adsorption capacities for humic acid coated nanoparticles (24.13 mg/g) much higher than its uncoated counterpart (2.82 mg/g). Adsorption was process very fast and kinetics could be described with pseudo-second-order model (R2 > 0.98), for both nanoparticles. High E4/E6 ratio of extracted humic acid and Fourier transform infrared spectroscopy of coated nanoparticles (20–100 nm) indicated enrichment of hydroxyl, carboxylic, and aliphatic groups on surface leading for the better adsorption. Humic acid coated and uncoated nanoparticles regenerated with EDTA, NaOH, urea, Na2CO3, and NaCl treatments retained 35.90–59.67 and 26.37–36.28% of their initial adsorption capacities, respectively, in 2nd cycle. Experimental controls (virgin nanoparticles subjected to an identical regenerating environment) revealed irreversible surface modification as the cause for loss of their adsorption capacities.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Acosta-Rodríguez I, Cárdenas-González JF, de Guadalupe Moctezuma-Zárate M et al (2013) Removal of hexavalent chromium from solutions and contaminated sites by different natural biomasses. In: Patil YB, Rao P (eds) Applied bioremediation. IntechOpen, Rijeka
ASTM (2017) Standard test methods for chromium in water. ASTM, D1687–17, West Conshohocken
Baalousha M, Manciulea A, Cumberland S et al (2008) Aggregation and surface properties of iron oxide nanoparticles: influence of pH and natural organic matter. Environ Toxicol Chem 27:1875–1882. https://doi.org/10.1897/07-559.1
Babel S, Kurniawan TA (2004) Cr(VI) removal from synthetic wastewater using coconut shell charcoal and commercial activated carbon modified with oxidizing agents and/or chitosan. Chemosphere 54:951–967. https://doi.org/10.1016/J.CHEMOSPHERE.2003.10.001
Bai RS, Abraham TE (2003) Studies on chromium(VI) adsorption-desorption using immobilized fungal biomass. Bioresour Technol 87:17–26
Barakat MA (2011) New trends in removing heavy metals from industrial wastewater. Arab J Chem 4:361–377. https://doi.org/10.1016/J.ARABJC.2010.07.019
Burks T, Avila M, Akhtar F et al (2014) Studies on the adsorption of chromium(VI) onto 3-Mercaptopropionic acid coated superparamagnetic iron oxide nanoparticles. J Colloid Interface Sci 425:36–43. https://doi.org/10.1016/J.JCIS.2014.03.025
Chen Q, Yin D, Zhu S, Hu X (2012) Adsorption of cadmium(II) on humic acid coated titanium dioxide. J Colloid Interface Sci 367:241–248. https://doi.org/10.1016/j.jcis.2011.10.005
Crisostomo CAB, Lima FA, Dias RM et al (2016) Joint assessment of bioreduction of chromium(VI) and of removals of both total chromium and total organic carbon (TOC) in sequential hybrid bioreactors. Water Air Soil Pollut 227:51. https://doi.org/10.1007/s11270-016-2747-9
Deng L, Shi Z, Luo L et al (2014) Adsorption of hexavalent chromium onto kaolin clay based adsorbent. J Cent South Univ 21:3918–3926. https://doi.org/10.1007/s11771-014-2379-4
Enev V, Pospíšilová L, Klučáková M et al (2014) Spectral characterization of selected humic substances. Soil Water Res 9:9–17
Fong SS, Mohamed M (2007) Chemical characterization of humic substances occurring in the peats of Sarawak, Malaysia. Org Geochem 38:967–976. https://doi.org/10.1016/j.orggeochem.2006.12.010
Grossl PR, Eick M, Sparks DL, et al. (1997) Arsenate and chromate retention mechanisms on goethite. 2. Kinetic evaluation using a pressure-jump relaxation technique. https://doi.org/10.1021/ES950654L
Gupta VK, Rastogi A (2008) Sorption and desorption studies of chromium(VI) from nonviable cyanobacterium Nostoc muscorum biomass. J Hazard Mater 154:347–354. https://doi.org/10.1016/j.jhazmat.2007.10.032
Hammaini A, González F, Ballester A et al (2007) Biosorption of heavy metals by activated sludge and their desorption characteristics. J Environ Manag 84:419–426. https://doi.org/10.1016/j.jenvman.2006.06.015
He YT, Traina SJ (2005) Cr(VI) reduction and immobilization by magnetite under alkaline pH conditions: the role of passivation. Environ Sci Technol 39:4499–4504. https://doi.org/10.1021/es0483692
Helms JR, Stubbins A, Ritchie JD et al (2008) Absorption spectral slopes and slope ratios as indicators of molecular weight, source, and photobleaching of chromophoric dissolved organic matter. Limnol Oceanogr 53:955–969. https://doi.org/10.4319/lo.2008.53.3.0955
Hong-bo F, Xie Q, Shuo C et al (2005) Interaction of humic substances and hematite: FTIR study. J Environ Sci 17:43–47
Hu J, Lo IMC, Chen G (2004) Removal of Cr(VI) by magnetite nanoparticle. Water Sci Technol 50:139–146
Hu J-D, Zevi Y, Kou X-M et al (2010) Effect of dissolved organic matter on the stability of magnetite nanoparticles under different pH and ionic strength conditions. Sci Total Environ 408:3477–3489. https://doi.org/10.1016/j.scitotenv.2010.03.033
Illés E, Tombácz E (2006) The effect of humic acid adsorption on pH-dependent surface charging and aggregation of magnetite nanoparticles. J Colloid Interface Sci 295:115–123. https://doi.org/10.1016/j.jcis.2005.08.003
Jadidi M, Etesami N, Esfahany MN (2017) Adsorption and desorption processes of chromium ions using magnetic iron oxide nanoparticles and their relevant mechanism. Iran J Chem Eng 14:31–40
Javanshah A, Saidi A (2016) Determination of humic acid by spectrophotometric analysis in the soils. Int J Adv Biotechnol Res 7:19–23
Jiang W, Cai Q, Xu W et al (2014) Cr(VI) adsorption and reduction by humic acid coated on magnetite. Environ Sci Technol 48:8078–8085. https://doi.org/10.1021/es405804m
Koesnarpadi S, Santosa SJ, Siswanta D, Rusdiarso B (2015) Synthesis and characterization of magnetite nanoparticle coated humic acid (Fe3O4/HA). Procedia Environ Sci 30:103–108. https://doi.org/10.1016/J.PROENV.2015.10.018
Naiya TK, Singha B, Das SK (2011) FTIR study for the Cr(VI) removal from aqueous solution using rice waste. International Conference on Chemistry and Chemical Process-IPCBEE 10:114–119
Lamar RT, Olk DC, Mayhew L, Bloom PR (2014) A new standardized method for quantification of humic and fulvic acids in humic ores and commercial products. J AOAC Int 97:721–730. https://doi.org/10.5740/jaoacint.13-393
Lasheen MR, El-Sherif IY, El-Wakeel ST et al (2017) Heavy metals removal from aqueous solution using magnetite Dowex 50WX4 resin nanocomposite. J Mater Environ Sci 8:503–511
Liu J, Zhao Z, Jiang G (2008) Coating Fe3O4 magnetic nanoparticles with humic acid for high efficient removal of heavy metals in water. Environ Sci Technol 42:6949–6954. https://doi.org/10.1021/es800924c
Ma H, Hua L, Lian K, Ma X (2014) Adsorptive removal of trivalent chromium in aqueous solution using precipitate produced from aluminum tanning wastewater. Water Air Soil Pollut 225:1956. https://doi.org/10.1007/s11270-014-1956-3
Mahmood T, Saddique MT, Naeem A et al (2011) Comparison of different methods for the point of zero charge determination of NiO. Ind Eng Chem Res 50:10017–10023. https://doi.org/10.1021/ie200271d
Maity D, Agrawal DC (2007) Synthesis of iron oxide nanoparticles under oxidizing environment and their stabilization in aqueous and non-aqueous media. J Magn Magn Mater 308:46–55. https://doi.org/10.1016/J.JMMM.2006.05.001
Mustafa S, Dilara B, Nargis K et al (2002) Surface properties of the mixed oxides of iron and silica. Colloids Surf A Physicochem Eng Asp 205:273–282. https://doi.org/10.1016/S0927-7757(02)00025-0
Naiya TK, Singha B, Das SK (2011) FTIR study for the Cr(VI) removal from aqueous solution using rice waste. International Conference on Chemistry and Chemical Process-IPCBEE 10:114–119
Niu H, Zhang D, Zhang S et al (2011) Humic acid coated Fe3O4 magnetic nanoparticles as highly efficient Fenton-like catalyst for complete mineralization of sulfathiazole. J Hazard Mater 190:559–565. https://doi.org/10.1016/j.jhazmat.2011.03.086
Pirbazari A, Pargami N, Ashja N, Emami M (2015) Surfactant-coated tea waste: preparation, characterization and its application for methylene blue adsorption from aqueous solution. J Environ Anal Toxicol 05:310. https://doi.org/10.4172/2161-0525.1000310
Qin X, Liu F, Wang G, Huang G (2015) Adsorption of humic acid from aqueous solution by hematite: effects of pH and ionic strength. Environ Earth Sci 73:4011–4017. https://doi.org/10.1007/s12665-014-3686-7
Rashid M, Price NT, Gracia Pinilla MÁ, O’Shea KE (2017) Effective removal of phosphate from aqueous solution using humic acid coated magnetite nanoparticles. Water Res 123:353–360. https://doi.org/10.1016/j.watres.2017.06.085
Rizzuti AM, Newkirk CR, Wilson KA et al (2017) Biosorption of hexavalent chromium from aqueous solutions using highly characterised peats. 19. https://doi.org/10.19189/MaP.2016.OMB.248
Rosliza S, Ahmed OH, Susilawat K et al (2009) Simple and rapid method of isolating humic acids from tropical peat soils (Saprists). Am J Appl Sci 6:820–823. https://doi.org/10.3844/ajas.2009.820.823
Shaker MA, Albishri HM (2014) Dynamics and thermodynamics of toxic metals adsorption onto soil-extracted humic acid. Chemosphere 111:587–595. https://doi.org/10.1016/j.chemosphere.2014.04.088
Smičiklas ID, Milonjić SK, Pfendt P, Raičević S (2000) The point of zero charge and sorption of cadmium(II) and strontium(II) ions on synthetic hydroxyapatite. Sep Purif Technol 18:185–194. https://doi.org/10.1016/S1383-5866(99)00066-0
Stancheva KA, Bogdanov BI, Georgiev DP et al (2013) Spectrophotometric determination of hexavalent chromium content in commercial cement—an assessment of the optimal conditions for the analysis of chromium(VI). Eurasian J Anal Chem 8:10–16
Tang W-W, Zeng G-M, Gong J-L et al (2014) Impact of humic/fulvic acid on the removal of heavy metals from aqueous solutions using nanomaterials: a review. Sci Total Environ 468–469:1014–1027. https://doi.org/10.1016/j.scitotenv.2013.09.044
Wu Z, Zhao D (2011) Ordered mesoporous materials as adsorbents. Chem Commun 47:3332–3338. https://doi.org/10.1039/c0cc04909c
Xiao Z, Zhang H, Xu Y et al (2017) Ultra-efficient removal of chromium from aqueous medium by biogenic iron based nanoparticles. Sep Purif Technol 174:466–473. https://doi.org/10.1016/j.seppur.2016.10.047
Yavuz CT, Mayo JT, Yu WW et al (2006) Low-field magnetic separation of monodisperse Fe3O4 nanocrystals. Science 314:964–967. https://doi.org/10.1126/science.1131475
Zhang X, Zhang P, Wu Z et al (2013) Adsorption of methylene blue onto humic acid-coated Fe3O4 nanoparticles. Colloids Surf A Physicochem Eng Asp 435:85–90. https://doi.org/10.1016/J.COLSURFA.2012.12.056
Zhou J, Wang Y, Wang J et al (2016) Effective removal of hexavalent chromium from aqueous solutions by adsorption on mesoporous carbon microspheres. J Colloid Interface Sci 462:200–207. https://doi.org/10.1016/J.JCIS.2015.10.001
Acknowledgments
SGS thanks the management of KITS for extended support during her project.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
There are no conflicts of interest to declare
Additional information
Responsible editor: Tito Roberto Cadaval
Publisher’s note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Electronic supplementary material
ESM 1
(PNG 629 kb)
Analysis of nanoparticles using DLS showing intensity distribution profile
ESM 2
(JPG 182 kb)
FTIR analysis of Humic acid-coated iron-oxide nanoparticle before and after chromium adsorption
ESM 3
(JPG 172 kb)
Kinetics for the adsorption of Cr(VI) onto INP and HINP, (a) removal from aqueous phase as a function of time and (b) adopting the pseudo-second-order model
Rights and permissions
About this article
Cite this article
Singaraj, S.G., Mahanty, B., Balachandran, D. et al. Adsorption and desorption of chromium with humic acid coated iron oxide nanoparticles. Environ Sci Pollut Res 26, 30044–30054 (2019). https://doi.org/10.1007/s11356-019-06164-0
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-019-06164-0