For the first time, functionalized zero-valent iron/walnut shell composite (CS-WS-NZVI) was prepared by immobilizing zero-valent iron nanoparticles within walnut shell (WS) modifying with chitosan using liquid phase reduction method. Activity of CS-WS-NZVI was investigated using tetracycline (TC) as target pollutant. Batch experiments were carried out to determinate the effect of reactant concentration, pH value, solution temperature, and competitive anions. Results show that TC could be removed by physical adsorption and chemical reduction on CS-WS-NZVI in a short time with high removal rates (more than 99.02%) at the optimal experiment conditions. Then, scanning electron microscopy analysis reveals that nanoscale zero-valent iron (NZVI) was distributed dispersedly on CS-WS-NZVI without being oxidized, and the mean particle size was 30–100 nm. Characterization results of X-ray diffraction and Fourier transforms infrared spectra of CS-WS-NZVI revealed that the iron nanoparticles were successfully loaded on the surface of WS. LC-MS analysis of the treated solution showed that degradation products were mainly derived from TC after losses of some groups from the ring, and the CS-WS-NZVI can absorb both TC and its degradation products. Furthermore, degradation of TC using CS-WS-NZVI was found to follow the two-parameter pseudo-first order decay kinetics model. Overall, our results indicated that CS-WS-NZVI might be a promising functional material for TC wastewater remediation.
Get full access to this article
View all access options for this article.
References
1.
AltunT., and PehlivanE. (2012). Removal of Cr(VI) from aqueous solutions by modified walnut shells. Food Chem. 132, 693.
2.
Arancibia-MirandaN., BaltazarS.E., GarciaA., Munoz-LiraD., SepulvedaP., RubioM.A., and AltbirD. (2016). Nanoscale zero valent supported by Zeolite and Montmorillonite: Template effect of the removal of lead ion from an aqueous solution. J. Hazard. Mater. 301, 371.
3.
AshrafiM., Arab ChamjangaliM., BagherianG., and GoudarziN. (2017). Application of linear and non-linear methods for modeling removal efficiency of textile dyes from aqueous solutions using magnetic Fe3O4 impregnated onto walnut shell. Spectrochim. Acta A Mol. Biomol. Spectrosc. 171, 268.
4.
BikousiM., GeorgiouY., DarkopoulosC., et al. (2015). Synthesis and characterization of robust zero valent iron/mesoporous carbon composites and their applications in arsenic removal. Carbon, 93, 636.
5.
BuschJ., MeißnerT., PotthoffA., BleylS., GeorgiA., MackenzieK., TrabitzschR., WerbanU., and OswaldS.E. (2015). A field investigation on transport of carbon-supported nanoscale zero-valent iron (nZVI) in groundwater. J. Contam. Hydrol. 181, 59.
6.
CaroniA.L.P.F., de LimaC.R.M., PereiraM.R., and FonsecaJ.L.C. (2012). Tetracycline adsorption on chitosan: A mechanistic description based on mass uptake and zeta potential measurements. Colloids Surf. B Biointerfaces, 100, 222.
7.
ChenD., GaoB., WangH.Y., and YangK. (2016). Effective removal of high concentration of phosphate by starch-stabilized nanoscale zerovalent iron (SNZVI). J. Taiwan Inst. Chem, E, 61, 181.
8.
ChenH., LuoH.J., LanY.C., DongT.T., HuB.J., and WangY.P. (2011). Removal of tetracycline from aqueous solutions using polyvinylpyrrolidone (PVP-K30) modified nanoscale zero valent iron. J. Hazard. Mater. 192, 44.
9.
DalmázioI., AlmeidaM.O., AugustiR., and AlvesT.M.A. (2007). Monitoring the degradation of tetracycline by ozone in aqueous medium via atmospheric pressure ionization mass spectrometry. J. Am. Soc. Mass. Spectrom. 18, 679.
10.
DiaoZ.-H., XuX.-R., JiangD., KongL.-J., SunY.-X., HuY.-X., HaoQ.-W., and ChenH. (2016). Bentonite-supported nanoscale zero-valent iron/persulfate system for the simultaneous removal of Cr(VI) and phenol from aqueous solutions. Chem. Eng. J. 302, 213.
11.
DongH., GuanX., and LoI.M.C. (2012). Fate of As(V)-treated nano zero-valent iron: Determination of arsenic desorption potential under varying environmental conditions by phosphate extraction. Water Res. 46, 4071.
12.
DongH., ZhaoF., HeQ., XieY., ZengY., ZhangL., TangL., and ZengG. (2017). Physicochemical transformation of carboxymethyl cellulose-coated zero-valent iron nanoparticles (nZVI) in simulated groundwater under anaerobic conditions. Sep. Purif. Technol. 175, 376.
13.
FangZ., ChenJ., QiuX., QiuX., ChengW., and ZhuL. (2011). Effective removal of antibiotic metronidazole from water by nanoscale zero-valent iron particles. Desalination, 268, 60.
14.
FuY., PengL., ZengQ., YangY., SongH., ShaoJ., LiuS., and GuJ. (2015). High efficient removal of tetracycline from solution by degradation and flocculation with nanoscale zerovalent iron. Chem. Eng. J. 270, 631.
15.
GaoY., LiY., ZhangL., HuangH., HuJ., ShahS.M., and SuX. (2012). Adsorption and removal of tetracycline antibiotics from aqueous solution by graphene oxide. J. Colloid Interface Sci. 368, 540.
16.
HeF., and ZhaoD.Y. (2005). Preparation and characterization of a new class of starch-stabilized bimetallic nanoparticles for degradation of chlorinated hydrocarbons in water. Environ. Sci. Technol. 39, 3314.
17.
HomemV., and SantosL. (2011). Degradation and removal methods of antibiotics from aqueous matrices—A review. J. Environ. Manage. 92, 2304.
18.
HussainI., LiM., ZhangY., LiY., HuangS., DuX., LiuG., HayatW., and AnwarN. (2017). Insights into the mechanism of persulfate activation with nZVI/BC nanocomposite for the degradation of nonylphenol. Chem. Eng. J. 311, 163.
19.
JiaS.Y., YangZ., YangW.B., ZhangT.T., ZhangS.P., YangX.Z., DongY.Y., WuJ.Q., and WangY.P. (2016). Removal of Cu(II) and tetracycline using an aromatic rings-functionalized chitosan-based flocculant: Enhanced interaction between the flocculant and the antibiotic. Chem. Eng. J. 283, 495.
20.
KuangY., WangQ.P., ChenZ.L., MegharajM., and NaiduR. (2013). Heterogeneous Fenton-like oxidation of monochlorobenzene using green synthesis of iron nanoparticles. J. Colloid Interface Sci. 410, 67.
21.
LiH., GeY., and ZhangX. (2017). High efficient removal of lead from aqueous solution by preparation of novel PPG-nZVI beads as sorbents. Colloids Surf. Physicochem. Eng. Aspects, 513, 306.
22.
LinK., DingJ., and HuangX. (2012). Debromination of tetrabromobisphenol A by nanoscale zerovalent iron: Kinetics, influencing factors, and pathways. Ind. Eng. Chem. Res. 51, 8378.
23.
LiuT., WangZ.-L., ZhaoL., and YangX. (2012). Enhanced chitosan/Fe0-nanoparticles beads for hexavalent chromium removal from wastewater. Chem. Eng. J. 189, 196.
24.
LiuT., ZhaoL., SunD., and TanX. (2010). Entrapment of nanoscale zero-valent iron in chitosan beads for hexavalent chromium removal from wastewater. J. Hazard. Mater. 184, 724.
25.
LiuT.Y., YangY.L., WangZ.L., and SunY.Q. (2016). Remediation of arsenic(III) from aqueous solutions using improved nanoscale zero-valent iron on pumice. Chem. Eng. J. 288, 739.
26.
LuT., XuX., LiuX., and SunT. (2017). Super hydrophilic PVDF based composite membrane for efficient separation of tetracycline. Chem. Eng. J. 308, 151.
27.
LunaM., GastoneF., ToscoT., SethiR., VelimirovicM., GemoetsJ., MuyshondtR., SapionH., KlaasN., and BastiaensL. (2015). Pressure-controlled injection of guar gum stabilized microscale zerovalent iron for groundwater remediation. J. Contam. Hydrol. 181, 46.
28.
MarzbaliM.H., EsmaieliM., AbolghasemiH., and MarzbaliM.H. (2016). Tetracycline adsorption by H3PO4-activated carbon produced from apricot nut shells: A batch study. Process Saf. Environ. Prot. 102, 700.
29.
MuY., JiaF., AiZ., and ZhangL. (2017). Iron oxide shell mediated environmental remediation properties of nano zero-valent iron. Environ. Sci. Nano, 4, 27.
30.
OturanN., WuJ., ZhangH., SharmaV.K., and OturanM.A. (2013). Electrocatalytic destruction of the antibiotic tetracycline in aqueous medium by electrochemical advanced oxidation processes: Effect of electrode materials. Appl. Catal. B Environ. 140, 92.
31.
PonderS.M., DarabJ.G., and MalloukT.E. (2000). Remediation of Cr(VI) and Pb(II) aqueous solutions using supported, nanoscale zero-valent iron. Environ. Sci. Technol. 34, 2564.
32.
RimoldiL., MeroniD., CappellettiG., and ArdizzoneS. (2017). Green and low cost tetracycline degradation processes by nanometric and immobilized TiO2 systems. Catal. Today, 281, 38.
33.
SafinejadA., ChamjangaliM.A., GoudarziN., and BagherianG. (2017). Synthesis and characterization of a new magnetic bio-adsorbent using walnut shell powder and its application in ultrasonic assisted removal of lead. J. Environ. Chem. Eng. 5, 1429.
34.
ShiL.N., LinY.M., ZhangX., and ChenZ.L. (2011). Synthesis, characterization and kinetics of bentonite supported nZVI for the removal of Cr(VI) from aqueous solution. Chem. Eng. J. 171, 612.
35.
ShiZ.Q., FanD., JohnsonR.L., TratnyekP.G., NurmiJ.T., WuY.X., and WilliamsK.H. (2015). Methods for characterizing the fate and effects of nano zerovalent iron during groundwater remediation. J. Contam. Hydrol. 181, 17.
36.
SuH., FangZ., TsangP.E., FangJ., and ZhaoD. (2016a). Stabilisation of nanoscale zero-valent iron with biochar for enhanced transport and in-situ remediation of hexavalent chromium in soil. Environ. Pollut. 214, 94.
37.
SuH., FangZ., TsangP.E., ZhengL., ChengW., FangJ., and ZhaoD. (2016b). Remediation of hexavalent chromium contaminated soil by biochar-supported zero-valent iron nanoparticles. J. Hazard. Mater. 318, 533.
38.
WangC., LuoH., ZhangZ., WuY., ZhangJ., and ChenS. (2014). Removal of As(III) and As(V) from aqueous solutions using nanoscale zero valent iron-reduced graphite oxide modified composites. J. Hazard. Mater. 268, 124.
39.
WangX., LiuP., MaJ., and LiuH. (2017). Preparation of novel composites based on hydrophilized and functionalized polyacrylonitrile membrane-immobilized NZVI for reductive transformation of metronidazole. Appl. Surf. Sci. 396, 841.
40.
WangX.Y., DuY., and MaJ. (2016). Novel synthesis of carbon spheres supported nanoscale zero-valent iron for removal of metronidazole. Appl. Surf. Sci. 390, 50.
41.
WangX.Y., WangP., MaJ., LiuH.L., and NingP. (2015). Synthesis, characterization, and reactivity of cellulose modified nano zero-valent iron for dye discoloration. Appl. Surf. Sci. 345, 57.
42.
WesselsJ.M., FordW.E., SzymczakW., and SchneiderS. (1998). The complexation of tetracycline and anhydrotetracycline with Mg2+ and Ca2+: A spectroscopic study. J. Phys. Chem. B, 102, 9323.
43.
XiaS.Q., GuZ.L., ZhangZ.Q., ZhangJ., and HermanowiczS.W. (2014). Removal of chloramphenicol from aqueous solution by nanoscale zero-valent iron particles. Chem. Eng. J. 257, 98.
44.
XiaZ., LiuH.L., WangS., MengZ.H., and RenN.Q. (2012). Preparation and dechlorination of a poly(vinylidene difluoride)-grafted acrylic acid film immobilized with Pd/Fe bimetallic nanoparticles for monochloroacetic acid. Chem. Eng. J. 200, 214.
45.
YangF.C., HeY.Y., SunS.Q., ChangY., ZhaF., and LeiZ.Q. (2016). Walnut shell supported nanoscale Fe0 for the removal of Cu(II) and Ni(II) ions from water. J. Appl. Polym. Sci. 133, 43304.
46.
YangJ., WangX., ZhuM., LiuH., and MaJ. (2014). Investigation of PAA/PVDF-NZVI hybrids for metronidazole removal: Synthesis, characterization, and reactivity characteristics. J. Hazard. Mater. 264, 269.
47.
YangZ., JiaS., ZhuoN., YangW., and WangY. (2015). Flocculation of copper(II) and tetracycline from water using a novel pH- and temperature-responsive flocculants. Chemosphere, 141, 112.
48.
ZhangD., YinJ., ZhaoJ., ZhuH., and WangC. (2015). Adsorption and removal of tetracycline from water by petroleum coke-derived highly porous activated carbon. J. Environ. Chem. Eng. 3, 1504.
Supplementary Material
Please find the following supplemental material available below.
For Open Access articles published under a Creative Commons License, all supplemental material carries the same license as the article it is associated with.
For non-Open Access articles published, all supplemental material carries a non-exclusive license, and permission requests for re-use of supplemental material or any part of supplemental material shall be sent directly to the copyright owner as specified in the copyright notice associated with the article.
