Sains Malaysiana 45(7)(2016): 1155–1167

Lead Adsorption Behaviours on Nanoscale Zero Valent Irons (nZVI) Coupled with Rice Husk MCM-41

(Kelakuan Penjerapan Plumbum ke atas Besi Bervalensi Sifar pada Skala Nano (nZVI) Berganding dengan Sekam Padi MCM-41)

C. KAEWBUDDEE^1,2,3, P. CHANPIWAT⁴, P. KIDKHUNTHOD⁵ & K. WANTALA^1,2,3*

¹Department of Chemical Engineering, Faculty of Engineering, Khon Kaen University

Khon Kaen 40002, Thailand

²Chemical Kinetics and Applied Catalysis Laboratory (CKCL), Faculty of Engineering,

Khon Kaen University, Khon Kaen 40002, Thailand

³Research Center for Environmental and Hazardous Substance Management (EHSM)

Faculty of Engineering, Khon Kaen University, Khon Kaen 40002, Thailand

⁴Environmental Research Institute, Chulalongkorn University, Bangkok 10330, Thailand

⁵Synchrotron Light Research Institute, Nakhon Ratchasima, 30000, Thailand

Received: 02 November 2015/Accessed: 23 January 2016

ABSTRACT

The aims of this work were to investigate the characteristics of nanoscale zero valent irons (nZVI) coupled with mesoporous materials (RH-MCM-41) adsorbent and to study the removal mechanisms of Pb (II) from synthetical solutions using full pictorial design batch experiments. Synthetic nZVI coupled with RH MCM-41 as Pb (II) adsorbent were characterized by XRD, TEM, BET and XANES. The results of XANES analyses confirmed the ability of RH-MCM-41 to prevent oxidations of Fe⁰ to Fe²⁺ and Fe³⁺. XANES results also verified the oxidation states of Pb (II). The solution pH was the most significant positive effect in controlling Pb (II) adsorption. The equilibrium and kinetic adsorption isotherms well fitted with the Langmuir isotherm. The pseudo-second order kinetic adsorption indicated that the adsorption process is the rate limiting step for Pb (II) removal. Furthermore, Langmuir-Hinshelwood confirmed the obvious Pb (II) adsorption at the active site of adsorbents. The reduction rate constant (kr = 5,000 mg/L.min) was higher than the adsorption rate constant (Kad = 0.0002 L/mg). Regarding the research results, four pathways including: reduction process, adsorption on FeOOH, adsorption on RH-MCM-41 and complex reaction between Fe and Pb ions were suggested for Pb (II) removal by nZVI coupled with RH-MCM-41.

Keywords: Adsorption mechanism; mesoporous material; nanoscale zero valent irons; Pb; XANES

ABSTRAK

Penyelidikan ini bertujuan untuk mengkaji ciri besi bervalensi sifar pada skala nano (nZVI) berganding dengan penjerap bahan mesoporous (RH-MCM-41) dan mengkaji mekanisme penyingkiran Pb (II) daripada larutan sistetik menggunakan uji kaji reka bentuk kelompok gambar penuh. Gabungan penjerap sintetik nZVI dengan RH MCM-41 sebagai Pb (II) telah dicirikan oleh XRD, TEM, BET dan XANES. Keputusan analisis XANES mengesahkan keupayaan RH-MCM-41 untuk mengelakkan pengoksidaan Fe⁰ kepada Fe²⁺ dan Fe³⁺. Keputusan XANES ini juga mengesahkan keadaan pengoksidaan Pb (II). Larutan PH adalah kesan positif yang paling penting dalam mengawal penjerapan Pb (II). Penjerapan isoterma keseimbangan dan kinetik juga sepadan dengan isoterma Langmuir. Penjerapan kinetik tertib pseudo-kedua menunjukkan bahawa proses penjerapan adalah langkah untuk mengehadkan kadar penyingkiran Pb (II). Tambahan pula, Langmuir-Hinshelwood mengesahkan penjerapan pasti Pb (II) di tapak bahan penjerap aktif. Kadar pengurangan berterusan (kr = 5000 mg/L.min) adalah lebih tinggi daripada kadar penjerapan pemalar (Kad = 0.0002 L/mg). Mengenai hasil penyelidikan, empat laluan termasuk: proses pengurangan, penjerapan pada FeOOH, penjerapan pada RH-MCM-41 dan tindak balas kompleks antara ion Fe dan Pb dicadangkan untuk penyingkiran Pb (II) oleh nZVI berganding dengan RH-MCM-41.

Kata kunci: Bahan mesoporos; besi bervalensi sifar pada skala nano; mekanisme penjerapan; Pb; XANES

REFERENCES

Ahn, S.C., Oh, S.Y. & Cha, D.K. 2008. Enhanced reduction of nitrate by zero-valent iron at elevated temperatures. Journal of Hazardous Materials 156(1-3): 17-22.

Artkla, S., Kim, W., Choi, W. & Wittayakun, J. 2009. Highly enhanced photocatalytic degradation of tetramethylammonium on the hybrid catalyst of titania and MCM-41 obtained from rice husk silica. Applied Catalysis B: Environmental 91(1- 2): 157-164.

ATSDR 2007. Toxicological Profile: Lead. http://www.atsdr. cdc.gov/toxprofiles/tp.asp?id=96&tid=22. Accessed on 7 July 2015.

Babel, S. & Kurniawan, T.A. 2003. Low-cost adsorbents for heavy metals uptake from contaminated water: A review. Journal of Hazardous Materials 97(1-3): 219-243.

Bhatnagar, A., Vilar, V.J.P., Botelho, C.M.S. & Boaventura, R.A.R. 2011. A review of the use of red mud as adsorbent for the removal of toxic pollutants from water and wastewater. Environmental Technology 32(3): 231-249.

Boparai, H.K., Joseph, M. & O’Carroll, D.M. 2013. Cadmium (Cd2+) removal by nano zerovalent iron: surface analysis, effects of solution chemistry and surface complexation modeling. Environmental Science and Pollution Research 20(9): 6210-6221.

Case Studies in Environmental Medicine (CSEM): Lead toxicity. 2010. U.S. Department of Human Services, Public Health Service, Agency for Toxic Substance and Disease Registry (ATSDR).

Cechinel, M.A.P., Ulson de Souza, S.M.A.G. & Ulson de Souza, A.A. 2014. Study of lead (II) adsorption onto activated carbon originating from cow bone. Journal of Cleaner Production 65: 342-349.

Centers for Disease Control and Prevention. 2005. Preventing lead poisoning in young children. Atlanta: the Centers for Disease Control and Prevention.

Chand, P. & Pakade, Y.B. 2013. Removal of Pb from water by adsorption on apple pomace: equilibrium, kinetics, and thermodynamics studies. Journal of Chemistry 2013: e164575.

Dada, A.O., Olalekan, A.P., Olatunya, A.M. & DADA, O. 2012. Langmuir, Freundlich, Temkin and Dubinin-Radushkevich isotherms studies of equilibrium sorption of Zn2+ unto phosphoric acid modified rice husk. IOSR Journal of Applied Chemistry 3(1): 38-45.

Feng, N. & Guo, X. 2012. Characterization of adsorptive capacity and mechanisms on adsorption of copper, lead and zinc by modified orange peel. Transactions of Nonferrous Metals Society of China 22(5): 1224-1231.

Feng, Q., Lin, Q., Gong, F., Sugita, S. & Shoya, M. 2004. Adsorption of lead and mercury by rice husk ash. Journal of Colloid and Interface Science 278(1): 1-8.

Hwang, Y.H., Kim, D.G. & Shin, H.S. 2011. Mechanism study of nitrate reduction by nano zero valent iron. Journal of Hazardous Materials 185(2-3): 1513-1521.

Jiang, M., Jin, X., Lu, X.Q. & Chen, Z. 2010. Adsorption of Pb(II), Cd(II), Ni(II) and Cu(II) onto natural kaolinite clay. Desalination 252(1-3): 33-39.

Kim, S.A., Kamala-Kannan, S., Lee, K.J., Park, Y.J., Shea, P.J. & Lee, W.H. 2013. Removal of Pb(II) from aqueous solution by a zeolite–nanoscale zero-valent iron composite. Chemical Engineering Journal 217: 54-60.

Krasae, N., Wantala, K., Tantriratna, P. & Grisdanurak, N. 2014. Removal of nitrate by bimetallic copper-nanoscale zero-valent iron. Applied Environmental Research 36(2): 15-23.

Kržišnik, N., Mladenovič, A., Škapin, A.S., Škrlep, L., Ščančar, J. & Milačič, R. 2014. Nanoscale zero-valent iron for the removal of Zn2+, Zn(II)–EDTA and Zn(II)–citrate from aqueous solutions. Science of the Total Environment 476- 477: 20-28.

Kumar, K.V., Porkodi, K. & Rocha, F. 2008. Langmuir– Hinshelwood kinetics - A theoretical study. Catalysis Communications 9(1): 82-84.

Liang, W., Dai, C., Zhou, X. & Zhang, Y. 2014. Application of zero-valent iron nanoparticles for the removal of aqueous zinc ions under various experimental conditions. PLoS ONE 9(1): e85686.

Li, X. & Zhang, W. 2007. Sequestration of metal cations with zerovalent iron nanoparticles - a study with high resolution x-ray photoelectron spectroscopy (HR-XPS). The Journal of Physical Chemistry C 111(19): 6939-6946.

Lu, Y., He, J. & Luo, G. 2013. An improved synthesis of chitosan bead for Pb(II) adsorption. Chemical Engineering Journal 226: 271-278.

Melo, R.A.A., Giotto, M.V., Rocha, J. & Urquieta-González, E.A. 1999. MCM-41 ordered mesoporous molecular sieves synthesis and characterization. Materials Research 2(3): 173-179.

Naiya, T.K., Bhattacharya, A.K., Mandal, S. & Das, S.K. 2009. The sorption of lead(II) ions on rice husk ash. Journal of Hazardous Materials 163(2-3): 1254-1264.

Notification of Ministry of Industry Thailand, No 12, B.E. 2542. 1999. Royal Government Gazette. 112 Part 29D (under the Groundwater Act, B.E. 2520 (1977)).

Occupational Knowledge International. 2010, 2012. Summary of mass lead poisoning incidents. Occupational Knowledge International (OK International).

Oh, Y.J., Song, H., Shin, W.S., Choi, S.J. & Kim, Y.H. 2007. Effect of amorphous silica and silica sand on removal of chromium(VI) by zero-valent iron. Chemosphere 66(5): 858-865.

Onweremadu, E.U. 2008. Physico-chemical characterization of a farmland affected by wastewater in relation to heavy metals. Journal of Zhejiang University SCIENCE A 9(3): 366-372.

Pojananukij, N., Wantala, K., Neramittapapong, S. & Neramittapapong, A. 2016. Equilibrium, kinetics, and mechanism of lead adsorption using zero-valent iron coated on diatomite. Desalination and Water Treatment 57(39): 18475-18489.

Ponder, S.M., Darab, J.G. & Mallouk, T.E. 2000. Remediation of Cr(VI) and Pb(II) aqueous solutions using supported, nanoscale zero-valent iron. Environmental Science & Technology 34(12):   2564-2569.

Şengil, İ. A. & Özacar, M. 2009. Competitive biosorption of Pb²⁺, Cu2+ and Zn²⁺ ions from aqueous solutions onto valonia tannin resin. Journal of Hazardous Materials 166(2-3): 1488-1494.

Sonmezay, A., Öncel, M.S. & Bektas, N. 2012. Adsorption of lead and cadmium ions from aqueous solutions using manganoxide minerals. Transactions of Nonferrous Metals Society of China 22(12): 3131-3139.

Sun, C.J., Sun, L.Z. & Sun, X.X. 2013. Graphical evaluation of the favorability of adsorption processes by using conditional Langmuir constant. Industrial & Engineering Chemistry Research 52(39): 14251-14260.

Sun, Y.P., Li, X., Cao, J., Zhang, W. & Wang, H.P. 2006. Characterization of zero-valent iron nanoparticles. Advances in Colloid and Interface Science 120(1-3): 47-56.

Suwannaruang, T., Rivera, K.K.P., Neramittagapong, A. & Wantala, K. 2015. Effects of hydrothermal temperature and time on uncalcined TiO2 synthesis for reactive red 120 photocatalytic degradation. Surface and Coatings Technology 271: 192-200.

Tanboonchuy, V., Hsu, J.C., Grisdanurak, N. & Liao, C.H. 2011. Gas-bubbled nano zero-valent iron process for high concentration arsenate removal. Journal of Hazardous Materials 186(2-3): 2123-2128.

Wan, M.W., Kan, C.C., Rogel, B.D. & Dalida, M.L.P. 2010. Adsorption of copper (II) and lead (II) ions from aqueous solution on chitosan-coated sand. Carbohydrate Polymers 80(3): 891-899.

Wantala, K., Khamjumphol, C., Thananukool, N. & Neramittagapong, A. 2015. Degradation of reactive Red 3 by heterogeneous Fenton-like process over iron-containing RH-MCM-41 assisted by UV irradiation. Desalination and Water Treatment 54(3): 699-706.

Wantala, K., Sthiannopkao, S., Srinameb, B., Grisdanurak, N., Kim, K.W. & Han, S. 2012a. Arsenic adsorption by Fe loaded on RH-MCM-41 synthesized from rice husk silica. Journal of Environmental Engineering 138(1): 119-128.

Wantala, K., Khongkasem, E., Khlongkarnpanich, N., Sthiannopkao, S. & Kim, K.W. 2012b. Optimization of As(V) adsorption on Fe-RH-MCM-41-immobilized GAC using Box-Behnken design: Effects of pH, loadings, and initial concentrations. Applied Geochemistry 27(5): 1027-1034.

Wantala, K., Sthiannopkao, S., Srinameb, B., Grisdanurak, N. & Kim, K.W. 2010. Synthesis and characterization of Fe- MCM-41 from rice husk silica by hydrothermal technique for arsenate adsorption. Environmental Geochemistry and Health 32(4): 261-266.

WHO|WHO Guidelines for drinking-water quality. 2011. WHO. http://www.who.int/water_sanitation_health/dwq/guidelines/ en/. Accessed on 7 July 2015.

Xu, P., Zeng, G.M., Huang, D.L., Lai, C., Zhao, M.H., Wei, Z., Li, N.J., Huang, C. & Xie, G.X. 2012. Adsorption of Pb(II) by iron oxide nanoparticles immobilized Phanerochaete chrysosporium: equilibrium, kinetic, thermodynamic and mechanisms analysis. Chemical Engineering Journal 203: 423-431.

Yan, W., Herzing, A.A., Kiely, C.J. & Zhang, W. 2010. Nanoscale zero-valent iron (nZVI): aspects of the core-shell structure and reactions with inorganic species in water. Journal of Contaminant Hydrology 118(3-4): 96-104.

Zhang, W. 2003. Nanoscale iron particles for environmental remediation: an overview. Journal of Nanoparticle Research 5(3-4): 323-332.

Zhang, X., Lin, S., Chen, Z., Megharaj, M. & Naidu, R. 2011. Kaolinite-supported nanoscale zero-valent iron for removal of Pb²⁺ from aqueous solution: Reactivity, characterization and mechanism. Water Research 45(11): 3481-3488.

Zhang, X., Lin, S., Lu, X.Q. & Chen, Z. 2010. Removal of Pb(II) from water using synthesized kaolin supported nanoscale zero-valent iron. Chemical Engineering Journal 163(3): 243-248.

Zhang, Y., Li, Y., Dai, C., Zhou, X. & Zhang, W. 2014. Sequestration of Cd(II) with nanoscale zero-valent iron (nZVI): Characterization and test in a two-stage system. Chemical Engineering Journal 244: 218-226.

Zhang, Y., Su, Y., Zhou, X., Dai, C. & Keller, A.A. 2013. A new insight on the core-shell structure of zerovalent iron nanoparticles and its application for Pb(II) sequestration. Journal of Hazardous Materials 263(Part 2): 685-693.

*Corresponding author; email: kitirote@kku.ac.th