Optimization and mechanism analysis of multi-solid wastes-based geopolymer using response surface methodology

Abstract

The escalating production of industrial solid waste, combined with the dwindling availability of natural resources, has intensified the focus on waste recycling. However, the heterogeneity and complexity of waste pose significant challenges to determining process parameters. In this study, burnt coal cinder (BCC), granite powder (GP), and high-calcium fly ash (Class-C FA) were used as raw materials, and the response surface methodology (RSM) and single-factor experiments were applied to optimize the process parameters for geopolymer preparation. The optimized precursor powder composition was determined to be a mass ratio of 1.6:0.9:7.3 for BCC, GP, and Class-C FA. The NaOH-precursor powder ratio and liquid–solid ratio were adjusted to 0.084 and 0.222, respectively. The curing condition was set at 80°C for 24 h. The resulting 28 d-aged multi-solid wastes-based geopolymer exhibited a high compressive strength of 61.34 MPa. The microstructure, mineral phase, and atomic bonding of geopolymers were investigated using X-ray diffraction (XRD), thermal analysis (TA), Fourier transform infrared spectroscopy (FTIR), and scanning electron microscopy with energy dispersive spectroscopy (SEM-EDS). Findings indicate that the compressive strength of geopolymer is most significantly influenced by the Class-C FA, followed by BCC. Furthermore, a minor addition of GP can optimize the structural density of the geopolymer. The Ca present in the Class-C FA participates in the geopolymerization, forming a hybrid N–(C)–A–S–H gel. RSM optimization facilitates the synergistic utilization of multi-solid wastes, ensuring an even distribution of gel and filler. This research establishes a theoretical framework for optimizing the preparation parameters of multi-solid wastes-based geopolymer and its subsequent applications; it holds significant scientific implications for the circular economy, resource transformation, and environmental conservation.

Keywords

multi-solid wastes / geopolymer / response surface methodology / process parameters / synergistic effect / Engineering / Chemical Engineering / Chemical Sciences / Physical Chemistry (incl. Structural)

References

[1] J.C. Lao, R.Y. Ma, L.Y. Xu, et al., Fly ash-dominated high-strength engineered/strain-hardening geopolymer composites (HS-EGC/SHGC): Influence of alkalinity and environmental assessment, J. Clean. Prod., 447(2024), art. No. 141182.

[2] MiaoC, LiangLX, ZhangF, et al. . Review of the fabrication and application of porous materials from silicon-rich industrial solid waste. Int. J. Miner. Metall. Mater., 2022, 293424.

[3] L.N. Assi, K. Carter, E. Deaver, and P. Ziehl, Review of availability of source materials for geopolymer/sustainable concrete, J. Clean. Prod., 263(2020), art. No. 121477.

[4] C.F. Xin, S.X. Bao, Y.M. Zhang, B. Chen, W. Ding, and W.G. Gan, Selective leaching mechanisms of zinc from industrial waste using hybrid acids: Sustainable synthesis of nano-ZnO, J. Environ. Manage., 373(2025), art. No. 123528.

[5] RodchomM, WimuktiwanP, SoongprasitK, AtongD, VichaphundS. Preparation and characterization of ceramic materials with low thermal conductivity and high strength using high-calcium fly ash. Int. J. Miner. Metall. Mater., 2022, 2981635.

[6] ZhangQ, LiuB, XiaoK, EkbergC, ZhangSG. Preparation and hydration of industrial solid waste—ccement blends: A review. Int. J. Miner. Metall. Mater., 2022, 29122106.

[7] B. Ren, Y.L. Zhao, H.Y. Bai, S.C. Kang, T.T. Zhang, and S.X. Song, Eco-friendly geopolymer prepared from solid wastes: A critical review, Chemosphere, 267(2021), art. No. 128900.

[8] HadiMNS, Al-AzzawiM, YuT. Effects of fly ash characteristics and alkaline activator components on compressive strength of fly ash-based geopolymer mortar. Constr. Build. Mater., 2018, 175: 41.

[9] A. Öz, B. Bayrak, E. Kavaz, et al., The radiation shielding and microstructure properties of quartzic and metakaolin based geopolymer concrete, Constr. Build. Mater., 342(2022), art. No. 127923.

[10] A.L. Almutairi, B.A. Tayeh, A. Adesina, H.F. Isleem, and A.M. Zeyad, Potential applications of geopolymer concrete in construction: A review, Case Stud. Constr. Mater., 15(2021), art. No. e00733.

[11] DingW, BaoSX, ZhangYM, et al. . Stepwise recycling of valuable metals from spent lithium-ion batteries based on in situ thermal reduction and ultrasonic-assisted water leaching. Green Chem., 2023, 25176652.

[12] W. Ding, S.X. Bao, Y.M. Zhang, et al., Sustainable regeneration of high-performance cathode materials from spent lithium-ion batteries through magnetic separation and coprecipitation, J. Clean. Prod., 438(2024), art. No. 140798.

[13] BaoSX, LuoYP, ZhangYM. Fabrication of green one-part geopolymer from silica-rich vanadium tailing via thermal activation and modification. Int. J. Miner. Metall. Mater., 2022, 291177.

[14] Y. Shao, S.L. Ma, S.Y. Li, D.Y. Chen, Z.Q. Zhang, and Q. Ren, Low carbon research in precast concrete based on the synergistic mechanism of red mud-ground granulated blast furnace slag powder, J. Clean. Prod., 439(2024), art. No. 140882.

[15] X.X. Zhou and J.M. Shen, Micromorphology and microstructure of coal fly ash and furnace bottom slag based light-weight geopolymer, Constr. Build. Mater., 242(2020), art. No. 118168.

[16] Z.M. Qiu, S.X. Bao, Y.M. Zhang, et al., Effect of Portland cement on the properties of geopolymers prepared from granite powder and fly ash by alkali-thermal activation, J. Build. Eng., 76(2023), art. No. 107363.

[17] M. Sarıdemir and S. Çelikten, Effect of high temperature, acid and sulfate on properties of alkali-activated lightweight aggregate concretes, Constr. Build. Mater., 317(2022), art. No. 125886.

[18] Z.F. Li, J. Zhang, S.C. Li, C.J. Lin, Y.F. Gao, and C. Liu, Feasibility of preparing red mud-based cementitious materials: Synergistic utilization of industrial solid waste, waste heat, and tail gas, J. Clean. Prod., 285(2021), art. No. 124896.

[19] ZhangJJ, ZhangXY, LiuB, EkbergC, ZhaoSZ, ZhangSG. Phase evolution and properties of glass ceramic foams prepared by bottom ash, fly ash and pickling sludge. Int. J. Miner. Metall. Mater., 2022, 293563.

[20] HuangMY, BaoSX, ZhangYM, LuoYP, XuXQ, YangSY. Calcium-activated geopolymer ceramics: Study of powder calcination and amorphous gel phases. J. Am. Ceram. Soc., 2023, 10663964.

[21] I.D.S. Dos Santos, S.X. Bao, and M.Y. Huang, Mechanical and microstructural properties analysis of one-part geopolymer based on burnt coal cinder replaced by metakaolin, J. Build. Eng., 76(2023), art. No. 107265.

[22] M.Y. Huang, S.X. Bao, Y.M. Zhang, Y.P. Luo, X.Q. Xu, and I.D.S. Dos Santos, The combined effects of calcium oxide and phosphate on burnt coal cinder-based cementitious materials, Constr. Build. Mater., 362(2023), art. No. 129720.

[23] JiaLX, HuangM, HuangMY, et al. . Preparation of granite powder-based geopolymer by synergistic action of calcination and phosphoric acid. J. Am. Ceram. Soc., 2024, 1071501.

[24] NadeemM, IlyasS, HaqEU, et al. . Improved water retention and positive behavior of silica based geopolymer utilizing granite powder. Silicon, 2022, 1452337.

[25] E.A. Azimi, M.A.A. Mohd Salleh, M.M. Al Bakri Abdullah, et al., Effect of NaOH molar concentration on microstructure and compressive strength of dolomite/fly ash-based geopolymers, Arch. Metall. Mater, (2021), p. 993.

[26] MohapatraSS, MishraJ, NandaB, PatroSK. A review on waste-derived alkali activators for preparation of geopolymer composite. Mater. Today Proc., 2022, 56: 440.

[27] D. Pushpalal, S. Danzandorj, N. Bayarjavkhlan, T. Nishiwaki, and K. Yamamoto, Compressive strength development and durability properties of high-calcium fly ash incorporated concrete in extremely cold weather, Constr. Build. Mater., 316(2022), art. No. 125801.

[28] HanjitsuwanS, HunpratubS, ThongbaiP, MaensiriS, SataV, ChindaprasirtP. Effects of NaOH concentrations on physical and electrical properties of high calcium fly ash geopolymer paste. Cem. Concr. Compos., 2014, 45: 9.

[29] B.W. Chong, R. Othman, R. Putra Jaya, et al., Design of experiment on concrete mechanical properties prediction: A critical review, Materials, 14(2021), No. 8, art. No. 1866.

[30] X.S. Shi, C. Zhang, X.Q. Wang, T. Zhang, and Q.Y. Wang, Response surface methodology for multi-objective optimization of fly ash-GGBS based geopolymer mortar, Constr. Build. Mater., 315(2022), art. No. 125644.

[31] L.Z. Guo, M. Zhou, X.Y. Wang, C. Li, and H.Q. Jia, Preparation of coal gangue-slag-fly ash geopolymer grouting materials, Constr. Build. Mater., 328(2022), art. No. 126997.

[32] M.G. Sá Ribeiro, M.G. Sá Ribeiro, P.F. Keane, M.R. Sardela, W.M. Kriven, and R.A. Sá Ribeiro, Acid resistance of metakaolin-based, bamboo fiber geopolymer composites, Constr. Build. Mater., 302(2021), art. No. 124194.

[33] R.B. Zhang, T. Liu, Y.M. Zhang, Z.L. Cai, and Y.Z. Yuan, Preparation of spent fluid catalytic cracking catalyst-metakaolin based geopolymer and its process optimization through response surface method, Constr. Build. Mater., 264(2020), art. No. 120727.

[34] A.S. Srinivasa, K. Swaminathan, and S.C. Yaragal, Microstructural and optimization studies on novel one-part geopolymer pastes by Box–Behnken response surface design method, Case Stud. Constr. Mater., 18(2023), art. No. e01946.

[35] PrabhaVC, RevathiV, Sivamurthy ReddyS. Ambient cured high calcium fly ash geopolymer concrete with dolomite powder. Eur. J. Environ. Civ. Eng., 2022, 26157857.

[36] ShiZG, ShiCJ, ZhangJ, WanS, ZhangZH, OuZH. Alkali–silica reaction in waterglass-activated slag mortars incorporating fly ash and metakaolin. Cem. Concr. Res., 2018, 108: 10.

[37] K.Y. Chen, D.Z. Wu, Z.L. Zhang, et al., Modeling and optimization of fly ash–slag-based geopolymer using response surface method and its application in soft soil stabilization, Constr. Build. Mater., 315(2022), art. No. 125723.

[38] Alipanahpour DilE, GhaediM, GhezelbashGR, AsfaramA, PurkaitMK. Highly efficient simultaneous biosorption of Hg²⁺, Pb²⁺ and Cu²⁺ by Live yeast Yarrowia lipolytica 70562 following response surface methodology optimization: Kinetic and isotherm study. J. Ind. Eng. Chem., 2017, 48: 162.

[39] MohammedBS, KhedVC, NuruddinMF. Rubbercrete mixture optimization using response surface methodology. J. Clean. Prod., 2018, 171: 1605.

[40] ÖzerA, GürbüzG, ÇalimliA, KörbahtiBK. Biosorption of copper(II) ions on enteromorpha prolifera: Application of response surface methodology (RSM). Chem. Eng. J., 2009, 1463377.

[41] Z.P. Li, D.G. Lu, and X.J. Gao, Optimization of mixture proportions by statistical experimental design using response surface method-A review, J. Build. Eng., 36(2021), art. No. 102101.

[42] Y. Zhang, Y. Wang, Z.G. Wu, Y.M. Lu, A.H. Kang, and P. Xiao, Optimal design of geopolymer grouting material for semiflexible pavement based on response surface methodology, Constr. Build. Mater., 306(2021), art. No. 124779.

[43] C.L. Wong, K.H. Mo, U.J. Alengaram, and S.P. Yap, Mechanical strength and permeation properties of high calcium fly ash-based geopolymer containing recycled brick powder, J. Build. Eng., 32(2020), art. No. 101655.

[44] B.H. Zhu, R.E. Yu, J.Y. Shang, X.Y. Xi, Y. Liu, and X.J. Zhu, The influence of NaOH concentration on the strength and microstructure of ceramic binders prepared from coal gangue through geopolymerization, Mater. Res. Express, 11(2024), No. 2, art. No. 025202.

[45] ZhangXY, LiCQ, ZhengSL, DiYH, SunZM. A review of the synthesis and application of zeolites from coal-based solid wastes. Int. J. Miner. Metall. Mater., 2022, 2911.

[46] L. Long, Y.M. Zhao, G.J. Lv, Y. Duan, X.B. Liu, and X.G. Jiang, Improving stabilization/solidification of MSWI fly ash with coal gangue based geopolymer via increasing active calcium content, Sci. Total Environ., 854(2023), art. No. 158594.

[47] P.G. He, Q.K. Wang, S. Fu, et al., Hydrothermal transformation of geopolymers to bulk zeolite structures for efficient hazardous elements adsorption, Sci. Total Environ., 767(2021), art. No. 144973.

[48] ÖztürkZ B, Atabeyİİ. Mechanical and microstructural characteristics of geopolymer mortars at high temperatures produced with ceramic sanitaryware waste. Ceram. Int., 2022, 48912932.

[49] S. Iftikhar, K. Rashid, E. Ul Haq, I. Zafar, F.K. Alqahtani, and M.I. Khan, Synthesis and characterization of sustainable geopolymer green clay bricks: An alternative to burnt clay brick, Constr. Build. Mater., 259(2020), art. No. 119659.

[50] Z.J. Yang, D. Zhang, C.Y. Fang, et al., Hydration mechanisms of alkali-activated cementitious materials with ternary solid waste composition, Materials, 15(2022), No. 10, art. No. 3616.

[51] A. Kadhim, M. Sadique, R. Al-Mufti, and K. Hashim, Long-term performance of novel high-calcium one-part alkali-activated cement developed from thermally activated lime kiln dust, J. Build. Eng., 32(2020), art. No. 101766.

[52] D.D. Burduhos Nergis, P. Vizureanu, A.V. Sandu, D.P. Burduhos Nergis, and C. Bejinariu, XRD and TG-DTA study of new phosphate-based geopolymers with coal ash or metakaolin as aluminosilicate source and mine tailings addition, Materials, 15(2021), No. 1, art. No. 202.

[53] AkbelenM, ÖzbayN. Influence of acid activation on hydrogen adsorption properties of analcime-rich tuff from Turkey. Turk. J. Chem., 2022, 4651565.

[54] P.J. Sánchez-Soto, E. Garzón, L. Pérez-Villarejo, G.N. Angelopoulos, and D. Eliche-Quesada, Mining wastes of an albite deposit as raw materials for vitrified mullite ceramics, Minerals, 11(2021), No. 3, art. No. 232.

[55] P. Jin, L. Li, Z.L. Li, W.Y. Du, M. Khan, and Z.J. Li, Using recycled brick powder in slag based geopolymer foam cured at ambient temperature: Strength, thermal stability and microstructure, Constr. Build. Mater., 452(2024), art. No. 139008.

[56] LiuMYJ, AlengaramUJ, SanthanamM, JumaatMZ, MoKH. Microstructural investigations of palm oil fuel ash and fly ash based binders in lightweight aggregate foamed geopolymer concrete. Constr. Build. Mater., 2016, 120: 112.

[57] Álvarez-AyusoE, QuerolX, PlanaF, et al. . Environmental, physical and structural characterisation of geopolymer matrixes synthesised from coal (co-)combustion fly ashes. J. Hazard. Mater., 2008, 1541–3175.

[58] D.W. Zhang, K.F. Zhao, F.Z. Xie, H. Li, and D.M. Wang, Effect of water-binding ability of amorphous gel on the rheology of geopolymer fresh pastes with the different NaOH content at the early age, Constr. Build. Mater., 261(2020), art. No. 120529.

RIGHTS & PERMISSIONS

University of Science and Technology Beijing