Кинетика сорбции органических красителей метиленового синего и малахитового зеленого на высокопористом углеродном материале

В статье целью исследований являлось определение важных параметров сорбции органических соединений – синтетических красителей метиленового синего (МС) и малахитового зеленого (МЗ), на мезопористом углероде (МПУ) из водных растворов в ограниченном объеме. Для используемого сорбента определены элементный состав и площадь поверхности по БЭТ по адсорбции азота, которая составила 2360 м²/г. Проведен анализ механизмов поглощения с помощью кинетических зависимостей и изотерм сорбции, для чего применялись эмпирические уравнения псевдо-первого и псевдо-второго порядка, Еловича и внутричастичной диффузии, а также уравнения Ленгмюра, Фрейндлиха, Дубинина–Радушкевича. В ходе кинетических исследований установлено, что равновесие наступает после 15 мин извлечения при величине адсорбционной емкости 2446,6 мг/г по МС и 2043,1 мг/г по МЗ. Следует отметить, что извлечение молекул красителей проходит преимущественно по смешанно-диффузионному механизму и контролируется реакцией второго порядка согласно модели псевдо-второго порядка. Энергия активации имеет значение 0,016 кДж/моль по молекулам МЗ и 0,013 кДж/моль для МС, что подтверждает физический механизм поглощения красителей. Таким образом, в ходе экспериментальных исследований подтверждена высокая эффективность разработанного сорбента для очистки водных систем от соединений органической природы. 

1. Salahuddin NA, EL-Daly HA, El Sharkawy RG, Nasr BT. Synthesis and efficacy of PPy/CS/GO nanocomposites for adsorption of ponceau 4R dye. Polymer. 2018;146:291-303. DOI: 10.1016/j.polymer.2018.04.053

2. Li H, Fan J, Shi Z, Lian M, Tian M, et al. Preparation and characterization of sulfonated grapheneenhanced poly (vinyl alcohol) composite hydrogel and its application as dye absorbent. Polymer. 2015;60:96-106. DOI: 10.1016/j.polymer.2014.12.069

3. Saleh TA, Muhammad AM, Tawabini B, Ali SA. Aminomethylphosphonate chelating ligand and octadecyl alkyl chain in a resin for simultaneous removal of Co(II) ions and organic contaminants. Journal of Chemical and Engineering Data. 2016;9(61):3377-3385. DOI: 10.1021/cs.jced.6b00475

4. Yao T, Guo S, Zeng C, Wang C, Zhang L. Investigation on efficient adsorption of cationic dyes on porous magnetic polyacrylamide microspheres. Journal of Hazardous Materials. 2015;292:90-97. DOI: 10.1016/j.jhazmat.2015.03.014

5. Jauris IM, Fagan SB, Adebayo MA, Machado FM. Adsorption of acridine orange and methylene blue synthetic dyes and anthracene on single wall carbon nanotubes: A first principle approach. Computational and Theoretical Chemistry. 2016;1076:42-50. DOI: 10.1016/j.comptc.2015.11.021

6. Dehghani MH, Mostofi M, Alimohammadi M, McKay G, Yetilmezsoy K, et al. High-performance removal of toxic phenol by single-walled and multi-walled carbon nanotubes: Kinetics, adsorption, mechanism and optimization studies. Journal of Industrial and Engineering Chemistry. 2016;35:63-74. DOI: 10.1016/j.jiec.2015.12.010

7. Dod R, Banerjee G, Saini DR. Removal of methylene blue (MB) dye from water environment by processed Jowar Stalk [Sorghum bicolor (L.) Moench] adsorbent. Clean Technologies and Environmental Policy. 2015;17:2349-2359. DOI:10.1007/s10098-015-0977-y

8. Gao M, Wang Z, Yang C, Ning J, Zhou Z, et al. Novel magnetic graphene oxide decorated with persimmon tannins for efficient adsorption of malachite green from aqueous solutions. Colloids and Surfaces A: Physicochemical and Engineering Aspects. 2019;566:48-57. DOI: 10.1016/j.colsurfa.2019.01.016

9. Gupta V, Sadegh H, Yari M, Ghoshekandi RS, Maazinejad B, et al. Removal of ammonium ions from wastewater: A short review in development of efficient methods. Global Journal of Environmental Science and Management. 2015;1:149. DOI: 10.7508/gjesm.2015.02.007

10. Gupta VK, Moradi O, Tyagi I, Agarwal S, Sadegh H, et al. Study on the removal of heavy metal ions from industry waste by carbon nanotubes: Effect of the surface modification: a review. Critical Reviews in Environmental Science and Technology. 2015;46:93-118. DOI: 10.1080/10643389.2015.1061874

11. Habeeb OA, Ramesh K, Ali GAM, Yunus RM. Experimental design technique on removal of hydrogen sulfide using CaO-eggshells dispersed onto palm kernel shell activated carbon: Experiment, optimization, equilibrium and kinetic studies. Journal Wuhan University of Technology, Materials Science Edition. 2017;32:305-320. DOI: 10.1007/s11595-017-1597-7

12. Borah L, Goswami M, Phukan P. Adsorption of methylene blue and eosin yellow using porous carbon prepared from tea waste: Adsorption equilibrium, kinetics and thermodynamics study. Journal of Environmental Chemical Engineering. 2015;3:1018-1028. DOI: 10.1016/j.jece.2015.02.013

13. Mohammadi A, Abdolvand H, Isfahani AP. Alginate beads impregnated with sulfonate containing calix[4]arene-intercalated layered double hydroxides: In situ preparation, characterization and methylene blue adsorption studies. International Journal of Biological Macromolecules. 2020;146:89-98. DOI: 10.1016/j.ijbiomac.2019.12.229

14. Junlapong K, Maijan P, Chaibundit C, Chantarak S. Effective adsorption of methylene blue by biodegradable superabsorbent cassava starch-based hydrogel. International Journal of Biological Macromolecules. 2020;158:258-264. DOI: 10.1016/j.ijbiomac.2020.04.247

15. Jabli M, Almalki S G, Agougui H. An insight into methylene blue adsorption characteristics onto functionalized alginate bio-polymer gel beads with λcarrageenan-calcium phosphate, carboxymethyl cellulose, and celite 545. International Journal of Biological Macromolecules. 2020;156:1091-1103. DOI: 10.1016/j.ijbiomac.2019.11.140

16. Marrakchi F, Ahmed MJ, Khanday WA, Asif M, Hameed BH. Mesoporous-activated carbon prepared from chitosan flakes via single-step sodium hydroxide activation for the adsorption of methylene blue. International Journal of Biological Macromolecules. 2017;98:233-239. DOI: 10.1016/j.ijbiomac.2017.01.119

17. Memetova A, Tyagi I, Suhas, Singh P, Mkrtchyan E, et al. Porous material based on modified carbon and the effect of pore size distribution on the adsorption of methylene blue dye from an aqueous solution. Environmental Science and Pollution Research. 2022;30(9): 22617-22630. DOI: 10.1007/s11356-022-23486-8

18. Mkrtchyan ES, Burakova IV, Burakov AE, Ananyeva OA, Dyachkova TP, et al. Synthesis of nanocomposite material based on graphene oxide modified with lignosulfonate. Liquid Crystals and their Application. 2022;22(3):38-48. DOI: 10.18083/LCAppl.2022.3.38

19. Mkrtchyan ES, Neskoromnaya EA, Burakova IV, Ananyeva OA, Revyakina NA, et al. Comparative analysis of the adsorption kinetics of the methylene blue dye on graphene aerogel and activated coconut carbon. Advanced Materials & Technologies. 2020;(4(20)):021-028. DOI: 10.17277/amt.2020.04.pp.021-028

20. Zhang Z, Xu L, Liu Y, Feng R, Zou T, et al. Efficient removal of methylene blue using the mesoporous activated carbon obtained from mangosteen peel wastes: Kinetic, equilibrium, and thermodynamic studies. Microporous and Mesoporous Materials. 2021;315: 110904. DOI: 10.1016/j.micromeso.2021.110904

21. Mu Y, Du H, He W, Ma H. Functionalized mesoporous magnetic biochar for methylene blue removal: Performance assessment and mechanism exploration. Diamond and Related Materials. 2022;121:108795. DOI: 10.1016/j.diamond.2021.108795

22. Jawad AH, Saber SEM, Abdulhameed AS, Reghioua A, ALOthman ZA, et al. Mesoporous activated carbon from mangosteen (Garcinia mangostana) peels by H3PO4 assisted microwave: Optimization, characterization, and adsorption mechanism for methylene blue dye removal. Diamond and Related Materials. 2022;129:109389. DOI: 10.1016/j.diamond.2022.109389

23. Burakov AE, Tyagi I, Burakova IV, Milyutin VV, Nekrasova NA. et al. Efficient removal of europium radionuclides from natural and seawater using mesoporous carbon-based material. Journal of Molecular Liquids. 2022;365:120092. DOI: 10.1016/j.molliq.2022.120092

24. Qiu H, Lu LV, Pan B, Zhang W, Zhang Q. Critical review in adsorption kinetic models. Journal of Zhejiang University Science A. 2009;5(10):716-724. DOI: 10.1631/jzus.A0820524

25. Ho Y-S. Second-order kinetic model for the sorption of cadmium onto tree fern: A comparison of linear and non-linear methods. Water Research. 2006;40(1):119-125. DOI 10.1016/j.watres.2005.10.040

26. Plazinski W, Dziuba J, Rudzinski W. Modeling of sorption kinetics: the pseudo-second order equation and the sorbate intraparticle diffusivity. Adsorption. 2013;19(5):1055-1064. DOI: 10.1007/s10450-013-9529-0

27. Naghizadeh A, Ghasemi F, Derakhshani E, Shahabi H. Thermodynamic, kinetic and isotherm studies of sulfate removal from aqueous solutions by graphene and graphite nanoparticles. Desalination and Water Treatment. 2017;80:247-254. DOI: 10.5004/dwt.2017.20891

28. Van Loon GW, Duffy SJ. Environmental Chemistry. Second Edition. New York: Oxford University Press Inc.; 2017. 560 p.

29. Hutson ND, Yang RT. Theoretical basis for the Dubinin-Radushkevitch (D-R) adsorption isotherm equation. Adsorption. 1997;3:189-195. DOI: 10.1007/BF01650130