Effect of blast furnace slag substitution for cement in carbon-reduced and low-cost solidified/stabilized cementitious materials

Abstract

The development of low-carbon cementitious materials involves the selection of the appropriate raw materials and the transformation of the hydration mechanism. In this study, low-carbon and low-cost cementitious materials were prepared using municipal solid waste incineration fly ash (MSWI FA), blast furnace slag (BFS), and desulfurization gypsum (DFG) as raw materials to reduce clinker usage. Results showed that the compressive strength of K5 (mass ratio of BFS: DFG: MSWI FA = 7:1:2) after 360 d of curing was 41.49 MPa, with a low leaching concentration of heavy metal residues that meet groundwater Class II standards, a dioxin content of only 25 ngTEG/kg, and a stable pH value ranging between 11 and 11.5. Microscopic analysis revealed a continuous decrease in the Ca/Si atomic ratios of K4 (mass ratio of BFS: DFG: MSWI FA: P·I 42.5 = 42:10:20:28) and K5, i.e., 1.18–1.54 and 1.04–1.23, respectively, with the increase in the hydration age. The highest Al/Si atomic ratio of K5, i.e., 0.26–0.31, was observed with the strongest conversion trend of calcium–silicate–hydrate gel into calcium–aluminum–silicate–hydrate gel, and the network structure of sodium–(calcium)–aluminum–silicate–hydrate gel zeolite-like phase was generated. The water-to-binder (WTB) mass ratio of 0.35 was determined to be more suitable for the K4 and K5 systems and resulted in a 56.83% and 90.82% reduction in half-life t compared with the WTB ratio of 0.5, respectively. Notably, the value of the reaction velocity constant K in the induction period was 10 times that of K1, and the autocatalytic reaction controlled the value of N to < 1. The X-ray absorption near-edge structure indicated that Zn solidification produced Zn₂SiO₄ with a small solubility product. The production of 1 t of K5 emitted only 10.83 kg/t of CO₂, which was 40 times less than that of K1. Overall, K5 provides the highest economic benefit at 40.08 USD/t, and the clinker-free cementitious system with multisolid waste synergy has significant advantages in terms of solidifying harmful substances, reducing carbon emissions, and lowering costs.

Keywords

Low-carbon cementitious materials / Multisolid waste synergy / CO₂ emissions / Fly ash / Blast furnace slag / Desulfurization gypsum

References

[1] Y.Y. Zhang, L. Wang, L. Chen, B. Ma, Y.K. Zhang, W. Ni, D.C.W. Tsang, Treatment of municipal solid waste incineration fly ash: state-of-the-art technologies and future perspectives, J. Hazard. Mater. 411 (2021) 125132.

[2] H.X. Zhan, N. Mahyuddin, R. Sulaiman, F. Khayatian, Phase change material (PCM) integrations into buildings in hot climates with simulation access for energy performance and thermal comfort: a review, Constr. Build. Mater. 397 (2023) 132312.

[3] L. Wang, Y.Y. Zhang, L. Chen, B.L. Guo, Y.S. Tan, K. Sasaki, D.C.W. Tsang, Designing novel magnesium oxysulfate cement for stabilization/solidification of municipal solid waste incineration fly ash, J. Hazard. Mater. 423 (2022) 127025.

[4] R. Malviya, R. Chaudhary, Factors affecting hazardous waste solidification/stabilization: a review, J. Hazard. Mater. 137 (1) (2006) 267-276.

[5] Y. Su, J.M. Yang, D.B. Liu, S.C. Zhen, N.X. Lin, Y.X. Zhou, Effects of municipal solid waste incineration fly ash on solidification/stabilization of Cd and Pb by magnesium potassium phosphate cement, J. Environ. Chem. Eng. 4 (1) (2016) 259-265.

[6] M. Nag, T. Shimaoka, A novel and sustainable technique to immobilize lead and zinc in MSW incineration fly ash by using pozzolanic bottom ash, J. Environ. Manag. 329 (2023) 117036.

[7] N. Gineys, G. Aouad, D. Damidot, Managing trace elements in Portland cement-Part I: interactions between cement paste and heavy metals added during mixing as soluble salts, Cem. Concr. Compos. 32 (8) (2010) 563-570.

[8] X. He, Z.Y. Lai, T. Yan, J. Wu, Z.Y. Lu, S.Z. Lv, F. Li, X.L. Fan, Hydration characteristics and microstructure of magnesium phosphate cement in presence of Cu²⁺ , Constr. Build. Mater. 225 (2019) 234-242.

[9] L.N. Lu, C.Y. Xiang, Y.J. He, F.Z. Wang, S.G. Hu, Early hydration of C₃S in the presence of Cd²⁺, Pb²⁺ and Cr³⁺ and the immobilization of heavy metals in pastes , Constr. Build. Mater. 152 (2017) 923-932.

[10] N.W. Wiesława, T. Barbara, D. Sylwia, The properties of cement pastes and mortars processed with some heavy metal nitrates containing solutions, Procedia Eng. 108 (2015) 72-79.

[11] Q.Y. Chen, C.D. Hills, M. Tyrer, I. Slipper, H.G. Shen, A. Brough, Characterisation of products of tricalcium silicate hydration in the presence of heavy metals, J. Hazard. Mater. 147 (3) (2007) 817-825.

[12] L. Wang, D.A. Geddes, B. Walkley, J.L. Provis, V. Mechtcherine, D.C.W. Tsang, The role of zinc in metakaolin-based geopolymers, Cem. Concr. Res. 136 (2020) 106194.

[13] B.L. Guo, Y.S. Tan, L. Wang, L. Chen, Z.L. Wu, K. Sasaki, V. Mechtcherine, D.C.W. Tsang, High-efficiency and low-carbon remediation of zinc contaminated sludge by magnesium oxysulfate cement, J. Hazard. Mater. 408 (2021) 124486.

[14] L. Wang, L. Chen, D.C.W. Tsang, Y.Y. Zhou, J. Rinklebe, H. Song, E.E. Kwon, K. Baek, Y.S. Ok, Mechanistic insights into red mud, blast furnace slag, or metakaolin-assisted stabilization/solidification of arsenic-contaminated sediment, Environ. Int. 133 (2019) 105247.

[15] M.B. Ogundiran, H.W. Nugteren, G.J. Witkamp, Immobilisation of lead smelting slag within spent aluminate-fly ash based geopolymers, J. Hazard. Mater. 248-249 (2013) 29-36.

[16] M.T. Zhang, C.H. Yang, M. Zhao, K. Yang, R. Shen, Y.J. Zheng, Immobilization potential of Cr(VI) in sodium hydroxide activated slag pastes, J. Hazard. Mater. 321 (2017) 281-289.

[17] Y.Q. Liu, W.P. Zhu, E.H. Yang, Alkali-activated ground granulated blast-furnace slag incorporating incinerator fly ash as a potential binder, Constr. Build. Mater. 112 (2016) 1005-1012.

[18] C.C. Fan, B.M. Wang, H.M. Ai, Y. Qi, Z. Liu, A comparative study on solidification/stabilization characteristics of coal fly ash-based geopolymer and Portland cement on heavy metals in MSWI fly ash, J. Clean. Prod. 319 (2021) 128790.

[19] W. Zhang, X.M. Liu, Z.Q. Zhang, Y.T. Li, J.R. Gu, Y.G. Wang, Y. Xue, Circulating fluidized bed fly ash-blast furnace slag based cementitious materials: hydration behaviors and performance, Constr. Build. Mater. 342 (2022) 128006.

[20] E. Kapeluszna, Ł. Kotwica, A. Różycka, Ł. Gołek, Incorporation of Al in C-A-S-H gels with various Ca/Si and Al/Si ratio: microstructural and structural characteristics with DTA/TG, XRD, FTIR and TEM analysis, Constr. Build. Mater. 155 (2017) 643-653.

[21] X.M. Liu, X.B. Zhao, H.F. Yin, J.L. Chen, N. Zhang, Intermediate-calcium based cementitious materials prepared by MSWI fly ash and other solid wastes: Hydration characteristics and heavy metals solidification behavior, J. Hazard. Mater. 349 (2018) 262-271.

[22] G.R. Qian, X.Y. Yang, S.X. Dong, J.Z. Zhou, Y. Sun, Y.F. Xu, Q. Liu, Stabilization of chromium-bearing electroplating sludge with MSWI fly ash-based Friedel matrices, J. Hazard. Mater. 165 (1-3) (2009) 955-960.

[23] R.P.W.J. Struis, M. Pasquali, L. Borgese, A. Gianoncelli, M. Gelfi, P. Colombi, D. Thiaudière, L.E. Depero, G. Rizzo, E. Bontempi, Inertisation of heavy metals in municipal solid waste incineration fly ash by means of colloidal silica-a synchrotron X-ray diffraction and absorption study, RSC Adv. 3 (34) (2013) 14339-14351.

[24] F.M. Yang, X. Zhou, F.J. Pang, W.J. Wang, W.L. Wang, Z.M. Wang, Heavy metal removal of solid waste source sulphoaluminate cement with graphene oxide, Constr. Build. Mater. 303 (2021) 124460.

[25] T. El-Hasan, M. Harfouche, A. Aldrabee, N. Abdelhadi, N. Abu-Jaber, G. Aquilanti, Synchrotron XANES and EXAFS evidences for Cr⁺⁶ and V⁺⁵ reduction within the oil shale ashes through mixing with natural additives and hydration process , Heliyon 7 (4) (2021) e06769.

[26] Y.C. Dai, G.R. Qian, Y.L. Cao, Y. Chi, Y.F. Xu, J.Z. Zhou, Q. Liu, Z.P. Xu, S.Z. Qiao, Effective removal and fixation of Cr(VI) from aqueous solution with Friedel’s salt, J. Hazard. Mater. 170 (2-3) (2009) 1086-1092.

[27] J. Sun, L. Wang, J.J. Yu, B.L. Guo, L. Chen, Y.Y. Zhang, D.W. Wang, Z.X. Shen, D.C.W. Tsang, Cytotoxicity of stabilized/solidified municipal solid waste incineration fly ash, J. Hazard. Mater. 424 (2022) 127369.

[28] J. Li, S.Q. Zhang, Q. Wang, W. Ni, K.Q. Li, P.F. Fu, W.T. Hu, Z.F. Li, Feasibility of using fly ash-slag-based binder for mine backfilling and its associated leaching risks, J. Hazard. Mater. 400 (2020) 123191.

[29] S.Q. Zhang, T.Y. Shi, W. Ni, K.Q. Li, W. Gao, K. Wang, Y.Y. Zhang, The mechanism of hydrating and solidifying green mine fill materials using circulating fluidized bed fly ash-slag-based agent, J. Hazard. Mater. 415 (2021) 125625.

[30] C. Chen, G. Habert, Y. Bouzidi, A. Jullien, A. Ventura, LCA allocation procedure used as an incitative method for waste recycling: An application to mineral additions in concrete, Resour. Conserv. Recycl. 54 (12) (2010) 1231-1240.

[31] A. Paulu, M. Vitvarová, V. Kočí, Quantifying the industry-wide symbiotic potential: LCA of construction and energy waste management in the Czech Republic, Sustain. Prod. Consum. 34 (2022) 55-64.

[32] C. Li, S.P. Cui, Z.R. Nie, X.Z. Gong, Z.H. Wang, N. Itsubo, The LCA of Portland cement production in China, Int. J. Life Cycle Assess. 20 (1) (2015) 117-127.

[33] Y.Z. Cao, L.P. Guo, B. Chen, X.P. Fei, Modeling early age hydration kinetics and the hydrated phase of cement paste blended with chloride and sulfate, Constr. Build. Mater. 261 (2020) 120537.

[34] F. Pelisser, P.J.P. Gleize, A. Mikowski, Effect of the Ca/Si molar ratio on the micro/nanomechanical properties of synthetic C-S-H measured by nanoindentation, J. Phys. Chem. C 116 (32) (2012) 17219-17227.

[35] L. Black, A. Stumm, K. Garbev, P. Stemmermann, K.R. Hallam, G.C. Allen, X-ray photoelectron spectroscopy of the cement clinker phases tricalcium silicate and β-dicalcium silicate, Cem. Concr. Res. 33 (10) (2003) 1561-1565.

[36] X. Wang, W. Ni, J.J. Li, S.Q. Zhang, M. Hitch, R. Pascual, Carbonation of steel slag and gypsum for building materials and associated reaction mechanisms, Cem. Concr. Res. 125 (2019) 105893.

[37] B.G. Ma, X.H. Liu, H.B. Tan, T. Zhang, J.P. Mei, H.H. Qi, W.B. Jiang, F.B. Zou, Utilization of pretreated fly ash to enhance the chloride binding capacity of cement-based material, Constr. Build. Mater. 175 (2018) 726-734.

[38] J.W. Wang, Z.L. Hu, Y. Chen, J.L. Huang, Y.F. Ma, W.W. Zhu, J.P. Liu, Effect of Ca/Si and Al/Si on micromechanical properties of C(-A)-S-H, Cem. Concr. Res. 157 (2022) 106811.

[39] J.H. Huo, B.S. Yu, Z.G. Peng, Z.S. Wu, L.H. Zhang, Thermal control effects and mechanism of slag and fly ash on heat development of cement slurry used in hydrate formation, J. Nat. Gas Sci. Eng. 91 (2021) 103967.

[40] L. Liu, P. Yang, B. Zhang, C. Huan, L.J. Guo, Q.X. Yang, K.I. Song, Study on hydration reaction and structure evolution of cemented paste backfill in early-age based on resistivity and hydration heat, Constr. Build. Mater. 272 (2021) 121827.

[41] J.P. Dai, Q.C. Wang, X.Y. Lou, X.Y. Bao, B. Zhang, J.Q. Wang, X. Zhang, Solution calorimetry to assess effects of water-cement ratio and low temperature on hydration heat of cement, Constr. Build. Mater. 269 (2021) 121222.

[42] J.G. Hamilton, R.E. Farrell, N. Chen, R.F. Feng, J. Reid, D. Peak, Characterizing zinc speciation in soils from a smelter-affected boreal forest ecosystem, J. Environ. Qual. 45 (2) (2016) 684-692.

[43] Y.S. Feng, Y.J. Du, A.N. Zhou, M. Zhang, J.S. Li, S.J. Zhou, W.Y. Xia, Geoenvironmental properties of industrially contaminated site soil solidified/stabilized with a sustainable by-product-based binder, Sci. Total Environ. 765 (2021) 142778.

[44] Y.J. Du, M.L. Wei, K.R. Reddy, H.L. Wu, Effect of carbonation on leachability, strength and microstructural characteristics of KMP binder stabilized Zn and Pb contaminated soils, Chemosphere 144 (2016) 1033-1042.

[45] A. Manceau, L. Charlet, M.C. Boisset, B. Didier, L. Spadini, Sorption and speciation of heavy metals on hydrous Fe and Mn oxides. From microscopic to macroscopic, Appl. Clay Sci. 7 (1-3) (1992) 201-223.

[46] S. Bai, X.C. Guan, G.Y. Li, Early-age hydration heat evolution and kinetics of Portland cement containing nano-silica at different temperatures, Constr. Build. Mater. 334 (2022) 127363.

[47] Z.P. Li, D.G. Lu, X.J. Gao, Analysis of correlation between hydration heat release and compressive strength for blended cement pastes, Constr. Build. Mater. 260 (2020) 120436.

[48] Z.H. Xu, J.M. Gao, Y.S. Zhao, S.J. Li, Z.H. Guo, X. Luo, G.F. Chen, Promoting utilization rate of ground granulated blast furnace slag (GGBS): incorporation of nanosilica to improve the properties of blended cement containing high volume GGBS, J. Clean. Prod. 332 (2022) 130096.

[49] X.J. Lyu, G. Yao, Z.M. Wang, Q. Wang, L. Li, Hydration kinetics and properties of cement blended with mechanically activated gold mine tailings, Thermochim. Acta 683 (2020) 178457.

[50] E. Sobiecka, A. Obraniak, B. Antizar-Ladislao, Influence of mixture ratio and pH to solidification/stabilization process of hospital solid waste incineration ash in Portland cement, Chemosphere 111 (2014) 18-23.

[51] U.A. Birnin-Yauri, F.P. Glasser, Friedel’s salt, Ca₂Al(OH)₆(Cl,OH)·2H₂O: Its solid solutions and their role in chloride binding , Cem. Concr. Res. 28 (12) (1998) 1713-1723.

[52] H.J. Li, H.H. Sun, X.C. Tie, X.J. Xiao, A new method to evaluate the hydraulic activity of Al-Si materials, Sci. China Ser. E Technol. Sci. 51 (2) (2008) 113-120.

[53] T.L. Barr, S. Seal, K. Wozniak, J. Klinowski, ESCA studies of the coordination state of aluminium in oxide environments, J. Chem. Soc. Faraday Trans. 93 (1) (1997) 181-186.

[54] P.K. Rasmussen, J.H. Sørensen, L.C. Hoang, B. Feddersen, F. Larsen, Notched connection in timber-concrete composite deck structures: a literature review on push-off experiments & design approaches, Constr. Build. Mater. 397 (2023) 131761.