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Preparation and characterization of P-type zeolite for adsorption of Cr3+, Ni2+, and Co2+

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Abstract

Acid-washed coal fly ash (AW-CFA) was subjected to wet grinding activation followed by hydrothermal crystallization to synthesize P zeolite (FAZ-P). The FAZ-P obtained at 120 °C for 24 h exhibited a maximum relative crystallinity of 93.15% and was employed for the adsorption of Cr3+, Ni2+, and Co2+ from aqueous solutions. The zeolitization of coal fly ash (CFA) leads to an increase in specific surface area to 44.00 m2/g, resulting in the formation of nano-sized P zeolite crystals with uniformly narrow fissures and sizes within the range of 10–30 nm. Adsorption experimental results indicate that FAZ-P exhibits maximum adsorption capacities of 49.03 mg/g for Cr3+, 22.20 mg/g for Ni2+, and 27.25 mg/g for Co2+. The adsorption equilibrium data for both mixed and single-metal ion solutions conform to the Langmuir model, with the affinity sequence for heavy metal ions being Cr3+  > Co2+  > Ni2+. The pseudo-first-order and pseudo-second-order kinetic models effectively described the adsorption behavior of Cr3+, Ni2+, and Co2+. Increasing the initial pH value of the solution significantly enhanced the adsorption capacity of the adsorbent for heavy metal ions. The removal mechanism of metal ions involves both adsorption and ion exchange processes. The thermodynamic parameters indicated that the adsorption process was spontaneous and endothermic.

Graphical Abstract

This study utilizes solid waste pollutant coal fly ash as a raw material, synthesizing coal fly ash-based P zeolite through wet mechanical grinding activation and hydrothermal crystallization. The synthesized zeolite exhibits excellent heavy metal adsorption performance, offering the potential for resource utilization of coal fly ash and sustainable industrial applications through waste-to-waste processing.

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Data are available from the authors upon request.

References

  • Al-Qodah Z, Al-Shannag M (2017) Heavy metal ions removal from wastewater using electrocoagulation processes: a comprehensive review. Sep Sci Technol 52:2649–2676

    CAS  Google Scholar 

  • Alvarez-Ayuso E, Garcia-Sanchez A, Querol X (2003) Purification of metal electroplating waste waters using zeolites. Water Res 37:4855–4862

    CAS  Google Scholar 

  • Ayangbenro AS, Babalola OO (2017) A new strategy for heavy metal polluted environments: a review of microbial biosorbents. Int J Environ Res Public Health 14(1):94

    Google Scholar 

  • Baroud G, Cayer E, Bohner M (2005) Rheological characterization of concentrated aqueous beta-tricalcium phosphate suspensions: the effect of liquid-to-powder ratio, milling time, and additives. Acta Biomater 1:357–363

    CAS  Google Scholar 

  • Barthomeuf D (1996) Basic zeolites: characterization and uses in adsorption and catalysis. Catal Rev-Sci Eng 38:521–612

    Google Scholar 

  • Bhatt A, Priyadarshini S, Mohanakrishnan AA, Abri A, Sattler M, Techapaphawit S (2019) Physical, chemical, and geotechnical properties of coal fly ash: A global review. Case Stud Constr Mater 11:e00263

  • Bukhari SS, Behin J, Kazemian H, Rohani S (2015) Conversion of coal fly ash to zeolite utilizing microwave and ultrasound energies: a review. Fuel 140:250–266

    CAS  Google Scholar 

  • De La Torre AG, Bruque S, Aranda MAG (2001) Rietveld quantitative amorphous content analysis. J Appl Crystallogr 34:196–202

    Google Scholar 

  • Deng H, Ge Y (2015) Formation of NaP zeolite from fused fly ash for the removal of Cu(II) by an improved hydrothermal method. RSC Adv 5:9180–9188

    CAS  Google Scholar 

  • Erdem E, Karapinar N, Donat R (2004) The removal of heavy metal cations by natural zeolites. J Colloid Interface Sci 280:309–314

    CAS  Google Scholar 

  • Erol K (2017a) Polychelated cryogels: hemoglobin adsorption from human blood. Artif Cells, Nanomed Biotechnol 45:31–38

    CAS  Google Scholar 

  • Erol K (2017b) The adsorption of calmoduline via nicotinamide immobilized poly (HEMA-GMA) cryogels. J Turk Chem Soc Sect: Chem 4:133–148

    CAS  Google Scholar 

  • Erol K, Uzun L (2017) Two-step polymerization approach for synthesis of macroporous surface ion-imprinted cryogels. J Macromol Sci, Part A 54:867–875

    CAS  Google Scholar 

  • Erol K, Yavuz Ş (2022) Invertase adsorption with polymers functionalized by aspartic acid. J Polym Eng 42:628–636

    CAS  Google Scholar 

  • Erol K, Gençer N, Arslan M, Arslan O (2013) Purification, characterization, and investigation of in vitro inhibition by metals of paraoxonase from different sheep breeds. Artif Cells, Nanomed Biotechnol 41:125–130

    CAS  Google Scholar 

  • Erol K, Yıldız E, Alacabey İ, Karabörk M, Uzun L (2019) Magnetic diatomite for pesticide removal from aqueous solution via hydrophobic interactions. Environ Sci Pollut Res 26:33631–33641

    Google Scholar 

  • Erol K, Bülter MB, Köse DA, Can HK (2021a) Water-soluble polymeric particle embedded cryogels: synthesis, characterisation and adsorption of haemoglobin. J Polym Eng 41:671–680

    CAS  Google Scholar 

  • Erol K, Tatar D, Veyisoğlu A, Tokatlı A (2021b) Antimicrobial magnetic poly (GMA) microparticles: synthesis, characterization and lysozyme immobilization. J Polym Eng 41:144–154

    CAS  Google Scholar 

  • Fernandez-Jimenez A, Palomo A (2005) Mid-infrared spectroscopic studies of alkali-activated fly ash structure. Microporous Mesoporous Mater 86:207–214

    CAS  Google Scholar 

  • Fu Z, Xi S (2020) The effects of heavy metals on human metabolism. Toxicol Mech Methods 30:167–176

    CAS  Google Scholar 

  • Georgi A, Kopinke F-D (2005) Interaction of adsorption and catalytic reactions in water decontamination processes: Part I. Oxidation of organic contaminants with hydrogen peroxide catalyzed by activated carbon. Appl Catal B 58:9–18

    CAS  Google Scholar 

  • Ghobarkar H, Schaf O, Guth U (1999) Zeolites - from kitchen to space. Prog Solid State Chem 27:29–73

    CAS  Google Scholar 

  • He K, Chen Y, Tang Z, Hu Y (2016) Removal of heavy metal ions from aqueous solution by zeolite synthesized from fly ash. Environ Sci Pollut Res 23:2778–2788

    CAS  Google Scholar 

  • Ho Y-S, McKay G (1999) Pseudo-second order model for sorption processes. Process Biochem 34:451–465

    CAS  Google Scholar 

  • Hui KS, Chao CYH, Kot SC (2005) Removal of mixed heavy metal ions in wastewater by zeolite 4A and residual products from recycled coal fly ash. J Hazard Mater 127:89–101

    CAS  Google Scholar 

  • Jakobsen BH (1998) K. H. Tan: Soil sampling, preparation, and analysis. Books in soil, plants, and the environment, 45. Dekker, New York 1996. xx, 408 s., ill, 24 cm. USD 100. Nova Hedwigia 93:363–373

    Google Scholar 

  • Joseph L, Jun B-M, Flora JRV, Park CM, Yoon Y (2019) Removal of heavy metals from water sources in the developing world using low-cost materials: a review. Chemosphere 229:142–159

    CAS  Google Scholar 

  • Kim S, Chu KH, Al-Hamadani YAJ, Park CM, Jang M, Kim D-H, Yu M, Heo J, Yoon Y (2018) Removal of contaminants of emerging concern by membranes in water and wastewater: a review. Chem Eng J 335:896–914

    CAS  Google Scholar 

  • Kireç O, Alacabey İ, Erol K, Alkan H (2021) Removal of 17β-estradiol from aqueous systems with hydrophobic microspheres. J Polym Eng 41:226–234

    Google Scholar 

  • Lagergren SK (1898) About the theory of so-called adsorption of soluble substances. Sven Vetenskapsakad Handingarl 24:1–39

    Google Scholar 

  • Langmuir I (1918) The adsorption of gases on plane surfaces of glass, mica and platinum. J Am Chem Soc 40:1361–1403

    CAS  Google Scholar 

  • Leinonen H, Lehto J (2001) Purification of metal finishing waste waters with zeolites and activated carbons. Waste Manage Res 19:45–57

    CAS  Google Scholar 

  • Li X, Ye J, Liu Z, Qiu Y, Li L, Mao S, Wang X, Zhang Q (2018) Microwave digestion and alkali fusion assisted hydrothermal synthesis of zeolite from coal fly ash for enhanced adsorption of Cd(II) in aqueous solution. J Central South Univ 25:9–20

    CAS  Google Scholar 

  • Liu Y, Wang G, Wang L, Li X, Luo Q, Na P (2019) Zeolite P synthesis based on fly ash and its removal of Cu (II) and Ni (II) ions. Chin J Chem Eng 27(2):341–348

    CAS  Google Scholar 

  • Lopez-Badillo CM, Lopez-Cuevas J, Gutierrez-Chavarria CA, Rodriguez-Galicia JL, Pech-Canul MI (2013) Synthesis and characterization of BaAl2Si2O8 using mechanically activated precursor mixtures containing coal fly ash. J Eur Ceram Soc 33:3287–3300

    CAS  Google Scholar 

  • Mainganye D, Ojumu TV, Petrik L (2013) Synthesis of zeolites Na-P1 from South African coal fly ash: effect of impeller design and agitation. Materials 6:2074–2089

    CAS  Google Scholar 

  • Mako E, Frost RL, Kristof J, Horvath E (2001) The effect of quartz content on the mechanochemical activation of kaolinite. J Colloid Interface Sci 244:359–364

    CAS  Google Scholar 

  • Mohebbi M, Rajabipour F, Scheetz BE (2017) Evaluation of two-atmosphere thermogravimetric analysis for determining the unburned carbon content in fly ash. Adv Civil Eng Mater 6:258–279

    CAS  Google Scholar 

  • Mondragon F, Rincon F, Sierra L, Escobar J, Ramirez J, Fernandez J (1990) New perspectives for coal ash utilization - synthesis of zeolitic materials. Fuel 69:263–266

    CAS  Google Scholar 

  • Murukutti MK, Jena H (2022) Synthesis of nano-crystalline zeolite-A and zeolite-X from Indian coal fly ash, its characterization and performance evaluation for the removal of Cs+ and Sr2+ from simulated nuclear waste. J Hazard Mater 423:127085

  • Namasivayam C, Yamuna RT, Jayanthi J (2003) Removal of methylene blue from wastewater by adsorption on cellulosic waste, orange peel. Cellul Chem Technol 37:333–339

    CAS  Google Scholar 

  • Nightingale ER (1959) Phenomenological theory of ion solvation - effective radii of hydrated ions. J Phys Chem 63:1381–1387

    CAS  Google Scholar 

  • Ouki SK, Kavannagh M (1997) Performance of natural zeolites for the treatment of mixed metal-contaminated effluents. Waste Manage Res 15:383–394

    CAS  Google Scholar 

  • Puligilla S, Mondal P (2015) Co-existence of aluminosilicate and calcium silicate gel characterized through selective dissolution and FTIR spectral subtraction. Cem Concr Res 70:39–49

    CAS  Google Scholar 

  • Ren X, Liu S, Qu R, Xiao L, Hu P, Song H, Wu W, Zheng C, Wu X, Gao X (2020) Synthesis and characterization of single-phase submicron zeolite Y from coal fly ash and its potential application for acetone adsorption. Micropor Mesopor Mater 295:109940

  • Shafiof MAS, Nezamzadeh-Ejhieh A (2020) A comprehensive study on the removal of Cd (II) from aqueous solution on a novel pentetic acid-clinoptilolite nanoparticles adsorbent: experimental design, kinetic and thermodynamic aspects. Solid State Sci 99:106071

  • Sivalingam S, Sen S (2019) Valorization of coal fly ash into nanozeolite by sonication-assisted hydrothermal method. J Environ Manage 235:145–151

    CAS  Google Scholar 

  • Tabit K, Waqif M, Saâdi L (2019) Application of the Taguchi method to investigate the effects of experimental parameters in hydrothermal synthesis of Na-P1 zeolite from coal fly ash. Res Chem Intermed 45:4431–4447

    CAS  Google Scholar 

  • Taty-Costodes VC, Fauduet H, Porte C, Delacroix A (2003) Removal of Cd(II) and Pb(II) ions, from aqueous solutions, by adsorption onto sawdust of Pinus sylvestris. J Hazard Mater 105:121–142

    CAS  Google Scholar 

  • Tauanov Z, Shah D, Inglezakis V, Jamwal PK (2018) Hydrothermal synthesis of zeolite production from coal fly ash: a heuristic approach and its optimization for system identification of conversion. J Clean Prod 182:616–623

    CAS  Google Scholar 

  • Tauanov Z, Azat S, Baibatyrova A (2022) A mini-review on coal fly ash properties, utilization and synthesis of zeolites. Int J Coal Prep Util 42:1968–1990

    CAS  Google Scholar 

  • Teğin İ, Akdeniz S, Alacabey İ, Erol K, Acar O (2023) Preconcentration and determination of Cu(II) and Cd(II) ions from wastewaters by using hazelnut shell biosorbent immobilized on Amberlite XAD-4 resin. MANAS J Eng. https://doi.org/10.51354/mjen.1260477

    Article  Google Scholar 

  • Tsai WT, Chen HP, Lai CW, Hsien KJ, Lee MS, Yang JM (2003) Preparation of adsorbents from sugarcane manufacturing by-product filter-mud by thermal activation. J Anal Appl Pyrol 70:399–411

    CAS  Google Scholar 

  • Wang S, Li L, Zhu ZH (2007) Solid-state conversion of fly ash to effective adsorbents for Cu removal from wastewater. J Hazard Mater 139:254–259

    CAS  Google Scholar 

  • Wang W, Feng Q, Liu K, Zhang G, Liu J, Huang Y (2015) A novel magnetic 4A zeolite adsorbent synthesised from kaolinite type pyrite cinder (KTPC). Solid State Sci 39:52–58

    CAS  Google Scholar 

  • Wu D, Sui Y, He S, Wang X, Li C, Kong H (2008) Removal of trivalent chromium from aqueous solution by zeolite synthesized from coal fly ash. J Hazard Mater 155:415–423

    CAS  Google Scholar 

  • Wu S, Han C, Xin L, Li M, Long H, Gao X (2023) Synthesis of triethylenetetramine modified sodium alginate/CuS nanocrystal composite for enhanced Cr(VI) removal: performance and mechanism. Int J Biol Macromol 238:124283

    CAS  Google Scholar 

  • Xu J, Cao Z, Zhang Y, Yuan Z, Lou Z, Xu X, Wang X (2018) A review of functionalized carbon nanotubes and graphene for heavy metal adsorption from water: preparation, application, and mechanism. Chemosphere 195:351–364

    CAS  Google Scholar 

  • Xu S, Pan D, Xiao G (2019) Enhanced HMF yield from glucose with H-ZSM-5 catalyst in water-tetrahydrofuran/2-butanol/2-methyltetrahydrofuran biphasic systems. J Central South Univ 26:2974–2986

    CAS  Google Scholar 

  • Yang L, Jiang T, Xiong P, Yang S, Gao M, Nagasaka T (2023) Green activating silica-alumina insoluble phase of fly ash to synthesize zeolite P with high adsorption capacity for Pb(II) in solution. Adv Powder Technol 34:103938

  • Ye Z, Yin X, Chen L, He X, Lin Z, Liu C, Ning S, Wang X, Wei Y (2019) An integrated process for removal and recovery of Cr(VI) from electroplating wastewater by ion exchange and reduction-precipitation based on a silica supported pyridine resin. J Clean Prod 236:117631

  • Yoldi M, Fuentes-Ordonez EG, Korili SA, Gil A (2019) Zeolite synthesis from industrial wastes. Microporous Mesoporous Mater 287:183–191

    CAS  Google Scholar 

  • Zeng R, Umana JC, Querol X, Lopez-Soler A, Plana F, Zhuang X (2002) Zeolite synthesis from a high Si-Al fly ash from East China. J Chem Technol Biotechnol 77:267–273

    CAS  Google Scholar 

  • Zhang Y, Kang W, Han H, Wang H, Chen Y, Gong X, Zhai C, Song H (2019) In-situ synthesis of NaP zeolite doped with transition metals using fly ash. J Am Ceram Soc 102:7665–7677

    CAS  Google Scholar 

  • Zhang Y, Chen Y, Kang W, Han H, Song H, Zhang C, Wang H, Yang X, Gong X, Zhai C, Deng J, Ai L (2020) Excellent adsorption of Zn(II) using NaP zeolite adsorbent synthesized from coal fly ash via stage treatment. J Clean Prod 258:120736

  • Zheng S, Wang Q, Yuan Y, Sun W (2020) Human health risk assessment of heavy metals in soil and food crops in the Pearl River Delta urban agglomeration of China. Food Chem 316:126213

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Funding

This work was supported by the Shandong Key Research and Development Plan (No. 2020CXGC011402) and the Shandong Province Natural Science Foundation (No. ZR2020ME190).

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All authors contributed to the study’s conception and design. Material preparation, data collection, and analysis were performed by Zhiyuan Liu and Xingxing Cheng. The first draft of the manuscript was written by Zhiyuan Liu, and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

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Correspondence to Xingxing Cheng.

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Highlights

• Mechanical grinding and alkali solutions produce synergistic activation of coal fly ash.

• Crystallization conditions can affect the relative crystallinity and phase purity of synthesized zeolites.

• The synthesized zeolite exhibits significantly higher surface area and pore volume compared to coal fly ash, offering increased adsorption sites for heavy metal removal.

• The removal mechanism of heavy metal ions by synthetic zeolite involves ion exchange and hydrous precipitation.

• The adsorption of heavy metal ions is an endothermic and spontaneous process.

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Liu, Z., Cheng, X. Preparation and characterization of P-type zeolite for adsorption of Cr3+, Ni2+, and Co2+. Environ Sci Pollut Res 31, 23664–23679 (2024). https://doi.org/10.1007/s11356-024-32623-4

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