Abstract
Herein, we report nickel oxide-decorated reduced graphene oxide synthesis through hydrothermal routes and their adsorption behavior in single and binary metal ion-containing aqueous media. The formation of the hybrid was verified through microscopic and spectroscopic characterizations. Generally, wastewater contains multiple metal ions, and the presence of other ions may affect the adsorption process. Hence, adsorption studies in a multicomponent system are essential to understand the adsorbent’s potential for real-life application. Systematic adsorption studied in single metal ion-containing solutions indicated that the hybrids’ adsorption capacities were ~ 725 mg g−1 and ~ 890 mg g−1 for cadmium and lead ion, respectively. Simultaneous metal ion removal experiments in binary metal ion systems indicated an increase in adsorption capacity with a maximum value of ~ 1000 mg g−1 for lead ion adsorption and a decrease in adsorption capacity with a maximum value of ~ 580 mg g−1 for cadmium ion adsorption. This observation suggested that the lead and cadmium ion adsorption process is affected by the synergistic and antagonistic effects, respectively. Experimental results indicate that the process followed the Langmuir isotherm and pseudo-second-order kinetics irrespective of the systems when the adsorption experiments were done in single and binary metal ion-containing systems. Thermodynamic studies indicated endothermicity and spontaneity of the process. The kinetic experiments showed that the film diffusion dominates the metal ion adsorption process.










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Ahmad MA, Alrozi R (2011) Removal of malachite green dye from aqueous solution using rambutan peel-based activated carbon: equilibrium, kinetic and thermodynamic studies. Chem Eng J 171(2):510–516. https://doi.org/10.1016/j.cej.2011.04.018
Alyüz B, Veli S (2009) Kinetics and equilibrium studies for the removal of nickel and zinc from aqueous solutions by ion exchange resins. J Hazard Mater 167(1):482–488. https://doi.org/10.1016/j.jhazmat.2009.01.006
Arshad F, Selvaraj M, Zain J, Banat F, Haija MA (2019) Polyethylenimine modified graphene oxide hydrogel composite as an efficient adsorbent for heavy metal ions. Sep Purif Technol 209:870–880. https://doi.org/10.1016/j.seppur.2018.06.035
Atia AA, Donia AM, Elwakeel KZ (2005) Adsorption behaviour of non-transition metal ions on a synthetic chelating resin bearing iminoacetate functions. Sep Purif Technol 43(1):43–48. https://doi.org/10.1016/j.seppur.2004.09.012
Behbahani M, Salarian M, Amini MM, Sadeghi O, Bagheri A, Bagheri S (2013) Application of a new functionalized nanoporous silica for simultaneous trace separation and determination of Cd(II), Cu(II), Ni(II), and Pb(II) in food and agricultural products. Food Anal Methods 6(5):1320–1329. https://doi.org/10.1007/s12161-012-9545-9
Biju V, Abdul Khadar M (2003) Fourier transform infrared spectroscopy study of nanostructured nickel oxide. Spectrochim Acta Part A Mol Biomol Spectrosc 59(1):121–134. https://doi.org/10.1016/S1386-1425(02)00120-8
Bunhu T, Tichagwa L, Chaukura N (2017) Competitive sorption of Cd2+ and Pb2+ from a binary aqueous solution by poly (methyl methacrylate)-grafted montmorillonite clay nanocomposite. Appl Water Sci 7(5):2287–2295. https://doi.org/10.1007/s13201-016-0404-5
Chen Y, Niu Y, Tian T, Zhang J, Wang Y, Li Y, Qin L-C (2017) Microbial reduction of graphene oxide by Azotobacter chroococcum. Chem Phys Lett 677:143–147. https://doi.org/10.1016/j.cplett.2017.04.002
Cui X, Yu X, Hou L, Gagnoud A, Fautrelle Y, Moreau R, Ren Z, Lu X, Li X (2016) Bismuth-based compounds crystals growth on graphene with various degrees of oxidation. J Alloys Compd 684:21–28. https://doi.org/10.1016/j.jallcom.2016.05.165
Deng X, Lü L, Li H, Luo F (2010) The adsorption properties of Pb(II) and Cd(II) on functionalized graphene prepared by electrolysis method. J Hazard Mater 183(1):923–930. https://doi.org/10.1016/j.jhazmat.2010.07.117
El-Korashy SA, Elwakeel KZ, El-Hafeiz AA (2016) Fabrication of bentonite/thiourea-formaldehyde composite material for Pb(II), Mn(VII) and Cr(VI) sorption: A combined basic study and industrial application. J Clean Prod 137:40–50. https://doi.org/10.1016/j.jclepro.2016.07.073
Elwakeel KZ, El-Bindary AA, Kouta EY (2017) Retention of copper, cadmium and lead from water by Na-Y-Zeolite confined in methyl methacrylate shell. J Environ Chem Eng 5(4):3698–3710. https://doi.org/10.1016/j.jece.2017.06.049
Elwakeel KZ, Aly MH, El-Howety MA, El-Fadaly E, Al-Said A (2018a) Synthesis of chitosan@activated carbon beads with abundant amino groups for capture of Cu(II) and Cd(II) from aqueous solutions. J Polym Environ 26(9):3590–3602. https://doi.org/10.1007/s10924-018-1243-2
Elwakeel KZ, El-Bindary AA, Kouta EY, Guibal E (2018b) Functionalization of polyacrylonitrile/Na-Y-zeolite composite with amidoxime groups for the sorption of Cu(II), Cd(II) and Pb(II) metal ions. Chem Eng J 332:727–736. https://doi.org/10.1016/j.cej.2017.09.091
Elwakeel KZ, Elgarahy AM, Khan ZA, Almughamisi MS, Al-Bogami AS (2020) Perspectives regarding metal/mineral-incorporating materials for water purification: with special focus on Cr(vi) removal. Mater Adv 1(6):1546–1574. https://doi.org/10.1039/D0MA00153H
Fu F, Wang Q (2011) Removal of heavy metal ions from wastewaters: a review. J Environ Manag 92(3):407–418. https://doi.org/10.1016/j.jenvman.2010.11.011
Gohel VD, Rajput A, Gahlot S, Kulshrestha V (2017) Removal of toxic metal ions from potable water by graphene oxide composites. Macromol Symp 376(1):1700050. https://doi.org/10.1002/masy.201700050
Hao L, Song H, Zhang L, Wan X, Tang Y, Lv Y (2012) SiO2/graphene composite for highly selective adsorption of Pb(II) ion. J Colloid Interface Sci 369(1):381–387. https://doi.org/10.1016/j.jcis.2011.12.023
Hobson JP (1969) Physical adsorption isotherms extending from ultrahigh vacuum to vapor pressure. J Phys Chem 73(8):2720–2727. https://doi.org/10.1021/j100842a045
Huang Z-H, Zheng X, Lv W, Wang M, Yang Q-H, Kang F (2011) Adsorption of lead(II) ions from aqueous solution on low-temperature exfoliated graphene nanosheets. Langmuir 27(12):7558–7562. https://doi.org/10.1021/la200606r
Jabeen H, Kemp KC, Chandra V (2013) Synthesis of nano zerovalent iron nanoparticles—graphene composite for the treatment of lead contaminated water. J Environ Manag 130:429–435. https://doi.org/10.1016/j.jenvman.2013.08.022
Karbarz M, Khalil AM, Wolowicz K, Kaniewska K, Romanski J, Stojek Z (2018) Efficient removal of cadmium and lead ions from water by hydrogels modified with cystine. J Environ Chem Eng 6(4):3962–3970. https://doi.org/10.1016/j.jece.2018.05.054
Li X, Zhou H, Wu W, Wei S, Xu Y, Kuang Y (2015) Studies of heavy metal ion adsorption on Chitosan/Sulfydryl-functionalized graphene oxide composites. J Colloid Interface Sci 448:389–397. https://doi.org/10.1016/j.jcis.2015.02.039
Liu Y, Gao C, Li Q, Pang H (2019) Nickel oxide/graphene composites: synthesis and applications. Chem Eur J 25(9):2141–2160. https://doi.org/10.1002/chem.201803982
Ma W, Ya F-Q, Han M, Wang R (2007) Characteristics of equilibrium, kinetics studies for adsorption of fluoride on magnetic-chitosan particle. J Hazard Mater 143(1):296–302. https://doi.org/10.1016/j.jhazmat.2006.09.032
Maity J, Ray SK (2018) Chitosan based nano composite adsorbent—synthesis, characterization and application for adsorption of binary mixtures of Pb(II) and Cd(II) from water. Carbohyd Polym 182:159–171. https://doi.org/10.1016/j.carbpol.2017.10.086
Malash GF, El-Khaiary MI (2010) Piecewise linear regression: a statistical method for the analysis of experimental adsorption data by the intraparticle-diffusion models. Chem Eng J (lausanne) 163(3):256–263. https://doi.org/10.1016/j.cej.2010.07.059
Mall ID, Srivastava VC, Agarwal NK, Mishra IM (2005) Adsorptive removal of malachite green dye from aqueous solution by bagasse fly ash and activated carbon-kinetic study and equilibrium isotherm analyses. Colloids Surf A 264(1):17–28. https://doi.org/10.1016/j.colsurfa.2005.03.027
Mirbagheri SA, Hosseini SN (2005) Pilot plant investigation on petrochemical wastewater treatmentfor the removal of copper and chromium with the objective of reuse. Desalination 171(1):85–93. https://doi.org/10.1016/j.desal.2004.03.022
Mishra SK, Tripathi SN, Choudhary V, Gupta BD (2014) SPR based fibre optic ammonia gas sensor utilizing nanocomposite film of PMMA/reduced graphene oxide prepared by in situ polymerization. Sens Actuators B Chem 199:190–200. https://doi.org/10.1016/j.snb.2014.03.109
Mouni L, Belkhiri L, Bollinger J-C, Bouzaza A, Assadi A, Tirri A, Dahmoune F, Madani K, Remini H (2018) Removal of Methylene Blue from aqueous solutions by adsorption on Kaolin: Kinetic and equilibrium studies. Appl Clay Sci 153:38–45. https://doi.org/10.1016/j.clay.2017.11.034
Nethravathi C, Rajamathi M (2008) Chemically modified graphene sheets produced by the solvothermal reduction of colloidal dispersions of graphite oxide. Carbon 46(14):1994–1998. https://doi.org/10.1016/j.carbon.2008.08.013
Oubagaranadin JUK, Sathyamurthy N, Murthy ZVP (2007) Evaluation of Fuller’s earth for the adsorption of mercury from aqueous solutions: a comparative study with activated carbon. J Hazard Mater 142(1):165–174. https://doi.org/10.1016/j.jhazmat.2006.08.001
Qi Y, Zhu L, Shen X, Sotto A, Gao C, Shen J (2019) Polythyleneimine-modified original positive charged nanofiltration membrane: Removal of heavy metal ions and dyes. Sep Purif Technol 222:117–124. https://doi.org/10.1016/j.seppur.2019.03.083
Ratna Kumar P, Chaudhari S, Khilar KC, Mahajan SP (2004) Removal of arsenic from water by electrocoagulation. Chemosphere 55(9):1245–1252. https://doi.org/10.1016/j.chemosphere.2003.12.025
Ren Y, Yan N, Feng J, Ma J, Wen Q, Li N, Dong Q (2012) Adsorption mechanism of copper and lead ions onto graphene nanosheet/δ-MnO2. Mater Chem Phys 136(2):538–544. https://doi.org/10.1016/j.matchemphys.2012.07.023
Rong X, Qiu F, Qin J, Zhao H, Yan J, Yang D (2015a) A facile hydrothermal synthesis, adsorption kinetics and isotherms to Congo Red azo-dye from aqueous solution of NiO/graphene nanosheets adsorbent. J Ind Eng Chem 26:354–363. https://doi.org/10.1016/j.jiec.2014.12.009
Rong X, Qiu F, Zhang C, Fu L, Wang Y, Yang D (2015b) Adsorption–photodegradation synergetic removal of methylene blue from aqueous solution by NiO/graphene oxide nanocomposite. Powder Technol 275:322–328. https://doi.org/10.1016/j.powtec.2015.01.079
Roy A, Bhattacharya J (2013) A binary and ternary adsorption study of wastewater Cd(II), Ni(II) and Co(II) by γ-Fe2O3 nanotubes. Sep Purif Technol 115:172–179. https://doi.org/10.1016/j.seppur.2013.05.010
Salam MA, Mokhtar M, Basahel SN, Al-Thabaiti SA, Obaid AY (2010) Removal of chlorophenol from aqueous solutions by multi-walled carbon nanotubes: kinetic and thermodynamic studies. J Alloys Compd 500(1):87–92. https://doi.org/10.1016/j.jallcom.2010.03.217
Saleh TA, Al-Saadi AA, Gupta VK (2014) Carbonaceous adsorbent prepared from waste tires: experimental and computational evaluations of organic dye methyl orange. J Mol Liq 191:85–91. https://doi.org/10.1016/j.molliq.2013.11.028
Salvestrini S, Leone V, Iovino P, Canzano S, Capasso S (2014) Considerations about the correct evaluation of sorption thermodynamic parameters from equilibrium isotherms. J Chem Thermodyn 68:310–316. https://doi.org/10.1016/j.jct.2013.09.013
Sangeetha K, Vidhya G, Vasugi G, Girija EK (2018) Lead and cadmium removal from single and binary metal ion solution by novel hydroxyapatite/alginate/gelatin nanocomposites. J Environ Chem Eng 6(1):1118–1126. https://doi.org/10.1016/j.jece.2018.01.018
Shahzad A, Miran W, Rasool K, Nawaz M, Jang J, Lim S-R, Lee DS (2017) Heavy metals removal by EDTA-functionalized chitosan graphene oxide nanocomposites. RSC Adv 7(16):9764–9771. https://doi.org/10.1039/C6RA28406J
Sheela T, Nayaka YA (2012) Kinetics and thermodynamics of cadmium and lead ions adsorption on NiO nanoparticles. Chem Eng J 191:123–131. https://doi.org/10.1016/j.cej.2012.02.080
Shen YF, Tang J, Nie ZH, Wang YD, Ren Y, Zuo L (2009) Preparation and application of magnetic Fe3O4 nanoparticles for wastewater purification. Sep Purif Technol 68(3):312–319. https://doi.org/10.1016/j.seppur.2009.05.020
Shivangi, Bhardwaj S, Sarkar T (2020) Core–shell type magnetic Ni/NiO nanoparticles as recyclable adsorbent for Pb (II) and Cd (II) ions: one-pot synthesis, adsorption performance, and mechanism. J Taiwan Inst Chem Eng 113:223–230. https://doi.org/10.1016/j.jtice.2020.08.011
Singh S, Barick KC, Bahadur D (2011) Surface engineered magnetic nanoparticles for removal of toxic metal ions and bacterial pathogens. J Hazard Mater 192(3):1539–1547. https://doi.org/10.1016/j.jhazmat.2011.06.074
Titelman GI, Gelman V, Bron S, Khalfin RL, Cohen Y, Bianco-Peled H (2005) Characteristics and microstructure of aqueous colloidal dispersions of graphite oxide. Carbon 43(3):641–649. https://doi.org/10.1016/j.carbon.2004.10.035
Wang L, Xing H, Gao S, Ji X, Shen Z (2017) Porous flower-like NiO@graphene composites with superior microwave absorption properties. J Mater Chem C 5(8):2005–2014. https://doi.org/10.1039/C6TC05179K
Xu H, Wu Y, Wang J, Shang X, Jiang X (2013) Simultaneous preconcentration of cadmium and lead in water samples with silica gel and determination by flame atomic absorption spectrometry. J Environ Sci 25:S45–S49. https://doi.org/10.1016/S1001-0742(14)60624-0
Yu W, Sisi L, Haiyan Y, Jie L (2020) Progress in the functional modification of graphene/graphene oxide: a review. RSC Adv 10(26):15328–15345. https://doi.org/10.1039/D0RA01068E
Zhang Y, Yan L, Xu W, Guo X, Cui L, Gao L, Wei Q, Du B (2014) Adsorption of Pb(II) and Hg(II) from aqueous solution using magnetic CoFe2O4-reduced graphene oxide. J Mol Liq 191:177–182. https://doi.org/10.1016/j.molliq.2013.12.015
Zhang K, Li H, Xu X, Yu H (2018) Synthesis of reduced graphene oxide/NiO nanocomposites for the removal of Cr(VI) from aqueous water by adsorption. Microporous Mesoporous Mater 255:7–14. https://doi.org/10.1016/j.micromeso.2017.07.037
Zheng Y, Zhu B, Chen H, You W, Jiang C, Yu J (2017) Hierarchical flower-like nickel(II) oxide microspheres with high adsorption capacity of Congo red in water. J Colloid Interface Sci 504:688–696. https://doi.org/10.1016/j.jcis.2017.06.014
Acknowledgements
Ms. Shivangi gratefully acknowledges the support from GGSIPU for IPRF fellowship and Tapan Sarkar is thankful to GGSIPU for the FRGS Grant [GGSIPU/DRC/FRGS/2018/31(1115)].
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S involved in methodology, formal analysis and investigation, and writing—original draft. SB involved in methodology, formal analysis, and investigation. TS involved in conceptualization, methodology, writing—review and editing, and supervision.
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Shivangi, Bhardwaj, S. & Sarkar, T. Simultaneous removal of cadmium and lead ions from aqueous solutions by nickel oxide-decorated reduced graphene oxides. Int. J. Environ. Sci. Technol. 19, 5595–5610 (2022). https://doi.org/10.1007/s13762-021-03510-z
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DOI: https://doi.org/10.1007/s13762-021-03510-z


