Abstract
Inorganic polymers (geopolymers) were synthesized by alkali activation of water treatment residue, a waste material containing aluminosilicates and a significant concentration of iron in the form of a ferric nanoparticle oxide gel. The effect on the structures of these geopolymers of incorporating the heavy metals chromium, zinc and iron, as occur in industrial wastewaters, was studied by their addition at the geopolymer synthesis stage, both as the pre-prepared hydroxides and as 1 M nitrate solutions. The heavy metals form several new crystalline phases, but the geopolymers display typical solid-state 27Al and 29Si MAS NMR characteristics. The 28-day strengths of the geopolymers without the metals (up to 11.2 MPa) were significantly degraded by the presence of the heavy metals, particularly 1 M zinc nitrate solution. The deleterious effect of the heavy metals on the strength may arise from their presence as the hydroxides rather than their incorporation as charge-balancing cations in the geopolymer structure. Leaching tests in simulated acid rain indicate that the geopolymers with molar ratios of SiO2/Al2O3 = 1.78 are capable of immobilizing all three metals to within safe leachate levels. The geopolymers are sufficiently strong to withstand handling and transportation and are capable of immobilizing wastes containing these heavy metals for storage or disposal.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Waijarean N, Asavapisit S, Sombatsompop K, MacKenzie KJD (2014) The effect of the Si/Al ratio on the properties of water treatment residue (WTR)-based geopolymers. Key Eng Mater 608:289–294
MacKenzie KJD (2009) Utilisation of non-thermally activated clays in the production of geopolymers. In: Provis JL, van Deventer JSJ (eds) Geopolymers: structure, processing, properties and industrial applications. Woodhead, Cambridge, p 294
Barbosa VFF, MacKenzie KJD, Thaumaturgo C (2000) Synthesis and characterisation of materials based on inorganic polymers of alumina and silica: sodium polysialate polymers. Int J Inorg Mater 2:309–317
Fletcher RA, MacKenzie KJD, Nicholson CL (2005) The composition range of aluminosilicate geopolymers. J Eur Ceram Soc 25:1471–1477
Cheng WT, Chiu PJ (2003) Fire-resistant geopolymer produced by granulated blast furnace slag. Miner Eng 16:205–210
Palomo A, Grutzek MW, Blanco MT (1999) Alkali-activated flyashes—a cement for the future. Cem Concr Res 29:1323–1329
Lemounga PN, MacKenzie KJD, Chinje Melo CF (2011) Synthesis and thermal properties of inorganic polymers (geopolymers) for structural and refractory applications from volcanic ash. Ceram Int 37:3011–3018
Hairi SNM, Jameson GNL, Rogers JJ, MacKenzie KJD (2015) Synthesis and properties of inorganic polymers (geopolymers) derived from Bayer process residue (red mud) and bauxite. J Mater Sci 50:7713–7724. doi:10.1007/s10853-015-9338-9
Temuujin J, Minjigmaa A, Davaabal B, Bayarzul U, Ankhtuya A, Ts Jadambaa, MacKenzie KJD (2014) Utilization of radioactive high-calcium Mongolian flyash for the preparation of alkali-activated geopolymers for safe use as construction materials. Ceram Int 40:16475–16483
Torgal FP, Castro Gomes JP, Jalali S (2007) Properties of tungsten mine waste geopolymeric binder. Constr Build Mater 22:1201–1211
Zheng L, Wang W, Shi Y (2010) The effects of alkaline dosage and Si/Al ratio on the immobilization of heavy metals in municipal; solid waste incineration fly ash-based geopolymer. Chemosphere 79:665–671
Waijarean N, Asavapisit S, Sombatsompop K (2014) Strength and microstructure of water treatment residue-based geopolymers containing heavy metals. Constr Build Mater 50:486–491
Van Jaarsveld JGS, Van Deventer FSJ (1999) The effect of metal contaminants on the formation and properties of waste-based geopolymers. Cem Concr Res 29:1189–1200
Provis JL (2009) Immobilisation of toxic wastes in geopolymers. In: Provis JL, van Deventer JSJ (eds) Geopolymers: structure, processing, properties and industrial applications. Woodhead, Cambridge, p 421
Zhang J, Provis JL, Feng D, Van Deventer JSJ (2008) Geopolymers for immobilization of Cr6+, Cd2+, and Pb2+. J Hazard Mater 157:587–598
Deja J (2002) Immobilization of Cr6+, Cd2+, Zn2+ and Pb2+ in alkali-activated slag binders. Cem Concr Res 32:1971–1979
Minarikova M, Skvara F (2006) Fixation of heavy metals in geopolymeric materials based on brown coal fly ash. Ceram Silik 50:200–207
Perera DS, Cashion JD, Blackford MG, Zhaoming Z, Vance ER (2007) Fe speciation in geopolymers with Si/Al molar ratio of 2. J Eur Ceram Soc 27:2697–2703
Bell JL, Kriven WM (2010) Formation of an iron-based inorganic polymer (geopolymer). In: Singh S, Kriven WM (eds) Mechanical properties and performance of engineering materials and composites IV. Wiley, Hoboken, pp 301–312
Lemougna PN, MacKenzie KJD, Jameson GNL, Rahier H, Chinje Melo UF (2013) The role of iron in the formation of inorganic polymers (geopolymers) from volcanic ash: a 57Fe Mössbauer spectroscopic study. J Mater Sci 48:5280–5286. doi:10.1007/s10853-013-7319-4
Hajimohammadi A, Provis JL, van Deventer JSJ (2011) Time-resolved and spatially resolved infrared spectroscopic observation of seeded nucleation controlling geopolymer gel formation. J Colloid Interface Sci 375:384–392
US Environmental Protection Agency SW-846 Test Method 1311, Toxicity Characteristic Leaching Procedure July 1992
MacKenzie KJD, Smith ME (2002) Multinuclear solid state NMR of inorganic materials, Pergamon materials series, vol 6. Pergamon/Elsevier, Oxford
MacKenzie KJD, Brown IWM, Cardile CM, Meinhold RH (1987) The thermal reactions of muscovite studied by high-resolution solid-state 29-Si and 27-Al NMR. J Mater Sci 22:2645–2654. doi:10.1007/BF01082158
Ennas G, Musinu A, Piccaluga G, Zedda D, Gatteschi D, Sangregorio C, Stanger JL, Concas G, Spano G (1998) Characterization of iron oxide nanoparticles in an Fe2O3–SiO2 composite prepared by a sol–gel method. Chem Mater 10:495–502
Rossano S, Behrens H, Wilke M (2008) Advanced analyses of 57Fe Mössbauer data of alumino-silicate glasses. Phys Chem Miner 35:77–93
Costa RCC, Moura FCC, Oliveira PEF, Maghalaes F, Ardisson JD, Largo RM (2010) Controlled reduction of red mud waste to produce active systems for environmental applications: heterogeneous Fenton reaction and reduction of Cr(VI). Chemosphere 78:1116–1120
Ramanaidou E, Nahorn D, Decarreau A, Melfi AJ (1996) Hematite and goethite from duricrusts developed by lateritic chemical weathering of precambrian banded iron formations, Minas Gerais, Brazil. Clays Clay Miner 44:22–31
Acknowledgements
This work is made possible by financial support from the Faculty of Science and Technology, Prince of Songkla University, Thailand. The assistance and advice of David Flynn and Olly Pantoja for assistance with the XRD and microstructural analyses is gratefully acknowledged, as is the assistance of the members of the Geopolymer Group of the MacDiarmid Institute for Advanced Materials and Nanotechnology where part of this work was carried out.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Waijarean, N., MacKenzie, K.J.D., Asavapisit, S. et al. Synthesis and properties of geopolymers based on water treatment residue and their immobilization of some heavy metals. J Mater Sci 52, 7345–7359 (2017). https://doi.org/10.1007/s10853-017-0970-4
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10853-017-0970-4