Chemical activation of phosphogypsum exhibits enhanced adsorption of malachite green from aqueous solution due to porosity refinement

Abstract

Owing to its uncomplicated synthetic methodology and exorbitant market demand, malachite green is widely used in numerous industries, particularly as a fungicide in aquaculture. Considering its intrinsic toxicity and potential long-term health impacts, deployable and cost-effective strategies must be developed for eliminating water-soluble malachite green. In this study, chemically activated phosphogypsum, a byproduct of fertilizer production, was used to remove malachite green from an aqueous system. Due to its low cost and abundance, the use of phosphogypsum as a sorbent material may significantly reduce the cost of adsorption-based processes. Moreover, its structural durability allows efficient recycling without significant deformation during reactivation. However, untreated phosphogypsum exhibits minimal efficiency in adsorbing synthetic dyes due to its unfavorable surface chemistry. Our investigation revealed that Zn activation induced a noticeable increase in pore volume from 0.03 to 0.06 cm³·g^–1. A 60 mg·L^–1 sorbent dose, pH 7, 150 r·min^–1, and operational temperature of 30 °C produced 99% quantitative sorption efficiency. Response surface methodology and artificial neural network were used to optimize process parameters by validating experimental values. No detectable toxicity was observed in Escherichia coli when exposed to the treated water.

Key words： malachite green; operating conditions optimization; phosphogypsum; sorption; water treatment

Competing interests

The authors declare that they have no competing interests.

Acknowledgements

This study was supported by the Ministry of Mines of the Government of India (Grant No. Met4-14/15/2022). Moonis Ali Khan acknowledges financial support through the Researchers Supporting Project (Grant No. RSP2024R345), King Saud University, Riyadh, Saudi Arabia. Ramesh Kumar acknowledges financial support through the Creative and Challenging Research Program (Grant No. 2021R1I1A1A01060846) of the National Research Foundation (NRF) of the Republic of Korea.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11705-024-2475-4 and is accessible for authorized users.

References

1 Bilalova S , Newig J , Tremblay-Lévesque L C , Roux J , Herron C , Crane S . Pathways to water sustainability? A global study assessing the benefits of integrated water resources management. Journal of Environmental Management, 2023, 343: 118179

2 Kumar R , Basu A , Bishayee B , Chatterjee R P , Behera M , Ang W L , Pal P , Shah M , Tripathy S K , Ambika S . . Management of tannery waste effluents towards the reclamation of clean water using an integrated membrane system: a state-of-the-art review. Environmental Research, 2023, 229: 115881

3 Kumar R , Liu C , Ha G S , Kim K H , Chakrabortty S , Tripathy S K , Park Y K , Khan M A , Yadav K K , Cabral-Pinto M M S . . A novel membrane-integrated sustainable technology for downstream recovery of molybdenum from industrial wastewater. Resources, Conservation and Recycling, 2023, 196: 107035

4 Kumar R , Awino E , Njeri D W , Basu A , Chattaraj S , Nayak J , Roy S , Khan G A , Jeon B H , Ghosh A K . . Advancing pharmaceutical wastewater treatment: a comprehensive review on application of catalytic membrane reactor-based hybrid approaches. Journal of Water Process Engineering, 2024, 58: 104838

5 Kumar R , Chakrabortty S , Chakrabortty P , Nayak J , Liu C , Ali Khan M , Ha G S , Ho Kim K , Son M , Roh H S . . Sustainable recovery of high-valued resources from spent lithium-ion batteries: a review of the membrane-integrated hybrid approach. Chemical Engineering Journal, 2023, 470: 144169

6 Jorge A M S , Athira K K , Alves M B , Gardas R L , Pereira J F B . Textile dyes effluents: a current scenario and the use of aqueous biphasic systems for the recovery of dyes. Journal of Water Process Engineering, 2023, 55: 104125

7 AbelA. 24-The history of dyes and pigments: from natural dyes to high performance pigments. In: Best J, editor. Colour Design (Second Edition). United Kingdom: Woodhead Publishing, 2012, 557–587

8 Kannaujiya M C , Kumar R , Mandal T , Mondal M K . Experimental investigations of hazardous leather industry dye (Acid Yellow 2GL) removal from simulated wastewater using a promising integrated approach. Process Safety and Environmental Protection, 2021, 155: 444–454

9 Alderman D J . Malachite green: a review. Journal of Fish Diseases, 1985, 8(3): 289–298

10 Gharavi-nakhjavani M S , Niazi A , Hosseini H , Aminzare M , Dizaji R , Tajdar-oranj B , Mirza Alizadeh A . Malachite green and leucomalachite green in fish: a global systematic review and meta-analysis. Environmental Science and Pollution Research International, 2023, 30(17): 48911–48927

11 Sharma J , Sharma S , Soni V . Toxicity of malachite green on plants and its phytoremediation: a review. Regional Studies in Marine Science, 2023, 62: 102911

12 Li T , Tian D , Zhu Z , Jin W , Wu S , Li H . The gut microbiota: a new perspective on the toxicity of malachite green (MG). Applied Microbiology and Biotechnology, 2019, 103(23–24): 9723–9737

13 Gopinathan R , Kanhere J , Banerjee J . Effect of malachite green toxicity on non target soil organisms. Chemosphere, 2015, 120: 637–644

14 Stammati A , Nebbia C , Angelis I D , Albo A G , Carletti M , Rebecchi C , Zampaglioni F , Dacasto M . Effects of malachite green (MG) and its major metabolite, leucomalachite green (LMG), in two human cell lines. Toxicology in Vitro, 2005, 19(7): 853–858

15 Zhou X , Zhang J , Pan Z , Li D . Review of methods for the detection and determination of malachite green and leuco-malachite green in aquaculture. Critical Reviews in Analytical Chemistry, 2019, 49(1): 1–20

16 Yaseen D A , Scholz M . Textile dye wastewater characteristics and constituents of synthetic effluents: a critical review. International Journal of Environmental Science and Technology, 2019, 16(2): 1193–1226

17 Oladoye P O , Ajiboye T O , Wanyonyi W C , Omotola E O , Oladipo M E . Insights into remediation technology for malachite green wastewater treatment. Water Science and Engineering, 2023, 16(3): 261–270

18 Umeh C T , Akinyele A B , Okoye N H , Emmanuel S S , Iwuozor K O , Oyekunle I P , Ocheje J O , Ighalo J O . Recent approach in the application of nanoadsorbents for malachite green (MG) dye uptake from contaminated water: a critical review. Environmental Nanotechnology, Monitoring & Management, 2023, 20: 100891

19 Joseph F , Agrawal Y K , Rawtani D . Behavior of malachite green with different adsorption matrices. Frontiers in Life Science, 2013, 7(3–4): 99–111

20 Naboulsi A , Himri M E , Gharibi E K , Haddad M E . Study of adsorption mechanism of malachite green (MG) and basic yellow 28 (BY28) onto smectite rich natural clays (Ghassoul) using DFT/B3LYP and DOE/FFD. Surfaces and Interfaces, 2022, 33: 102227

21 Chouaybi I , Moujahid E M , Bettach M . From waste to clean water: effective removal of Acid Red 97 dye using green synthesized hydrocalumite from phosphogypsum and aluminum foils. Inorganic Chemistry Communications, 2023, 158: 111653

22 Singh K , Kumar A , Singh A K , Agarwal A . Fly ash and TiO₂ modified fly ash as adsorbing materials for effective removal of methylene blue and malachite green from aqueous solutions. Journal of the Indian Chemical Society, 2023, 100(3): 100942

23 Muinde V M , Onyari J M , Wamalwa B , Wabomba J N . Adsorption of malachite green dye from aqueous solutions using mesoporous chitosan-zinc oxide composite material. Environmental Chemistry and Ecotoxicology, 2020, 2: 115–125

24 Bulut Y , Aydın H . A kinetics and thermodynamics study of methylene blue adsorption on wheat shells. Desalination, 2006, 194(1–3): 259–267

25 Zhang D , Wang B , Gong X , Yang Z , Liu Y . Selective reduction of nitrate to nitrogen gas by novel Cu₂O-Cu⁰@Fe⁰ composite combined with HCOOH under UV radiation. Chemical Engineering Journal, 2019, 359: 1195–1204

26 Basak B , Patil S , Kumar R , Ha G S , Park Y K , Ali Khan M , Kumar Yadav K , Fallatah A M , Jeon B H . Integrated hydrothermal and deep eutectic solvent-mediated fractionation of lignocellulosic biocomponents for enhanced accessibility and efficient conversion in anaerobic digestion. Bioresource Technology, 2022, 351: 127034

27 Dey P , Chakrabortty S , Haldar D , Sowmya A , Rangarajan V , Ruiz H A . Kinetic model supported improved and optimized submerged production strategy of cellulase enzyme from newspaper waste biomass. Bioprocess and Biosystems Engineering, 2022, 45(8): 1281–1295

28 Chowdhury S , Lahiri S K , Hens A , Katiyar S . Performance enhancement of commercial ethylene oxide reactor by artificial intelligence approach. International Journal of Chemical Reactor Engineering, 2022, 20(2): 237–250

29 Abumelha H M , Alzahrani S O , Alrefaee S H , Al-bonayan A M , Alkhatib F , Saad F A , El-Metwaly N M . Evaluation of tetracycline removal by magnetic metal organic framework from aqueous solutions: adsorption isotherm, kinetics, thermodynamics, and Box-Behnken design optimization. Journal of Saudi Chemical Society, 2023, 27(5): 101706

30 Singh T S , Pant K K . Equilibrium, kinetics and thermodynamic studies for adsorption of As(III) on activated alumina. Separation and Purification Technology, 2004, 36(2): 139–147

31 Saeed M , Munir M , Nafees M , Shah S S A , Ullah H , Waseem A . Synthesis, characterization and applications of silylation based grafted bentonites for the removal of Sudan dyes: isothermal, kinetic and thermodynamic studies. Microporous and Mesoporous Materials, 2020, 291: 109697

32 Iwasaki S , Koga N . Thermal dehydration of calcium sulfate dihydrate: physico-geometrical kinetic modeling and the influence of self-generated water vapor. Physical Chemistry Chemical Physics, 2020, 22(39): 22436–22450

33 Dantas H F , Mendes R A S , Pinho R D , Soledade L E B , Paskocimas C A , Lira B B , Schwartz M O E , Souza A G , Santos I M G . Characterizationof gypsum using TMDSC. Journal of Thermal Analysis and Calorimetry, 2007, 87(3): 691–695

34 Hammas-Nasri I , Horchani-Naifer K , Férid M , Barca D . Rare earths concentration from phosphogypsum waste by two-step leaching method. International Journal of Mineral Processing, 2016, 149: 78–83

35 Li X , Zhang Q . Hydration mechanism and hardening property of α-hemihydrate phosphogypsum. Minerals, 2019, 9(12): 733

36 Yuan E , Han W , Zhang G , Zhao K , Mo Z , Lu G , Tang Z . Structural and textural characteristics of Zn-containing ZSM-5 zeolites and application for the selective catalytic reduction of NO_x with NH₃ at high temperatures. Catalysis Surveys from Asia, 2016, 20(1): 41–52

37 Grabas K , Pawełczyk A , Stręk W , Szełęg E , Stręk S . Study on the properties of waste apatite phosphogypsum as a raw material of prospective applications. Waste and Biomass Valorization, 2019, 10(10): 3143–3155

38 Yorgun S , Vural N , Demiral H . Preparation of high-surface area activated carbons from Paulownia wood by ZnCl₂ activation. Microporous and Mesoporous Materials, 2009, 122(1-3): 189–194

39 Bellotto M , Artioli G , Dalconi M C , Corso R . On the preparation of concentrated gypsum slurry to reuse sulfate-process TiO₂ byproduct stream. Journal of Cleaner Production, 2018, 195: 1468–1475

40 van der MerweE MStrydomC APotgieterJ H. Thermogravimetric analysis of the reaction between carbon and CaSO₄·2H₂O, gypsum and phosphogypsum in an inert atmosphere. Thermochimica Acta, 1999, 340–341: 431–437

41 Das L , Sengupta S , Das P , Bhowal A , Bhattacharjee C . Experimental and numerical modeling on dye adsorption using pyrolyzed mesoporous biochar in batch and fixed-bed column reactor: isotherm, thermodynamics, mass transfer, kinetic analysis. Surfaces and Interfaces, 2021, 23: 100985

42 Salleh M A M , Mahmoud D K , Karim W A W A , Idris A . Cationic and anionic dye adsorption by agricultural solid wastes: a comprehensive review. Desalination, 2011, 280(1–3): 1–13

43 Zhou L , Jin J , Liu Z , Liang X , Shang C . Adsorption of acid dyes from aqueous solutions by the ethylenediamine-modified magnetic chitosan nanoparticles. Journal of Hazardous Materials, 2011, 185(2–3): 1045–1052

44 Mok C F , Ching Y C , Osman N A A , Muhamad F , Hai N D , Choo J H , Hassan C R . Adsorbents for removal of cationic dye: nanocellulose reinforced biopolymer composites. Journal of Polymer Research, 2020, 27(12): 373

45 Santhi T , Manonmani S , Smitha T . Removal of malachite green from aqueous solution by activated carbon prepared from the epicarp of Ricinus communis by adsorption. Journal of Hazardous Materials, 2010, 179(1–3): 178–186

46 Sarkar S , Tiwari N , Behera M , Chakrabortty S , Jhingran K , Sanjay K , Banerjee S , Tripathy S K . Facile synthesis, characterization and application of magnetic Fe₃O₄-coir pith composites for the removal of methyl violet from aqueous solution: kinetics, isotherm, thermodynamics and parametric optimization. Journal of the Indian Chemical Society, 2022, 99(5): 100447

47 Rafatullah M , Sulaiman O , Hashim R , Ahmad A . Removal of cadmium(II) from aqueous solutions by adsorption using meranti wood. Wood Science and Technology, 2012, 46(1–3): 221–241

48 Musah M , Azeh Y , Mathew J T , Umar M T , Abdulhamid Z , Muhammad A I . Adsorption kinetics and isotherm models: a review. Caliphate Journal of Science and Technology, 2022, 4(1): 20–26

49 Caianelo M , Rodrigues-Silva C , Maniero M G , Diniz V , Spina M , Guimarães J R . Evaluation of residual antimicrobial activity and acute toxicity during the degradation of gatifloxacin by ozonation. Water Science and Technology, 2021, 84(1): 225–236

50 Chakrabortty S , Pal M , Roy M , Pal P . Water treatment in a new flux-enhancing, continuous forward osmosis design: transport modelling and economic evaluation towards scale up. Desalination, 2015, 365: 329–342