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Acrylic acid grafted-multi-walled carbon nanotubes and their high-efficiency adsorption of methylene blue

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Abstract

A novel and simple method was explored to obtain (polyacrylic acid) PAA-g-MWCNTs by grafting acrylic acid (AA) onto the surface of the multi-walled carbon nanotubes (MWCNTs) using azobisisobutyronitrile (AIBN) as an initiator. The results of TEM, FTIR, XPS, Raman spectra and TG proved that AA is successfully grafted onto the surface of MWCNTs. Contact angle measurement and dispersion tests revealed that the hydrophilicity of PAA-g-MWCNTs is significantly higher than that of pretreated MWCNTs. The adsorption experiments of methylene blue (MB) showed that the adsorption capacity is proportional to the degree of functionalization and increases with initial concentration, pH and temperature. The maximum adsorption capacity is about 329.8 mg g−1. The kinetic and isothermal studies also showed that the adsorption data are consistent with pseudo-first-order and pseudo-second-order kinetic and Langmuir isothermal models. The remarkable adsorption capacity of PAA-g-MWCNTs can be attributed to the interaction of various adsorption mechanisms, and further analysis indicated that hydrogen bonding and electrostatic attraction play a decisive role in the adsorption process. In addition, the relationship between oxygen-containing groups content (OC) and MB adsorption capacity was revealed by a simulation using a mathematical model.

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References

  1. Ma J, Yu F, Zhou L, Jin L, Yang M, Luan J, Tang Y, Fan H, Yuan Z, Chen J (2012) Enhanced adsorptive removal of methyl orange and methylene blue from aqueous solution by alkali-activated multiwalled carbon nanotubes. ACS Appl Mater Interfaces 4(11):5749–5760

    Article  CAS  Google Scholar 

  2. Wu CH (2007) Adsorption of reactive dye onto carbon nanotubes: equilibrium, kinetics and thermodynamics. J Hazard Mater 144(1–2):93–100

    Article  CAS  Google Scholar 

  3. Yao Y, Xu F, Chen M, Xu Z, Zhu Z (2010) Adsorption behavior of methylene blue on carbon nanotubes. Bioresour Technol 101(9):3040–3046

    Article  CAS  Google Scholar 

  4. Mishra AK, Arockiadoss T, Ramaprabhu S (2010) Study of removal of azo dye by functionalized multi walled carbon nanotubes. Chem Eng J 162(3):1026–1034

    Article  CAS  Google Scholar 

  5. Cheng S, Zhang L, Ma A, Xia H, Peng J, Li C, Shu J (2018) Comparison of activated carbon and iron/cerium modified activated carbon to remove methylene blue from wastewater. J Environ Sci (China) 65:92–102

    Article  Google Scholar 

  6. El Hassani K, Kalnina D, Turks M, Beakou BH, Anouar A (2019) Enhanced degradation of an azo dye by catalytic ozonation over Ni-containing layered double hydroxide nanocatalyst. Sep Purif Technol 210:764–774

    Article  CAS  Google Scholar 

  7. Mohamed A, Ghobara MM, Abdelmaksoud MK, Mohamed GG (2019) A novel and highly efficient photocatalytic degradation of malachite green dye via surface modified polyacrylonitrile nanofibers/biogenic silica composite nanofibers. Sep Purif Technol 210:935–942

    Article  CAS  Google Scholar 

  8. Shi P, Hu X, Wang Y, Duan M, Fang S, Chen W (2018) A PEG-tannic acid decorated microfiltration membrane for the fast removal of Rhodamine B from water. Sep Purif Technol 207:443–450

    Article  CAS  Google Scholar 

  9. Othman N, Raja Sulaiman RN, Rahman HA, Noah NFM, Jusoh N, Idroas M (2019) Simultaneous extraction and enrichment of reactive dye using green emulsion liquid membrane system. Environ Technol 40(11):1476–1484

    Article  CAS  Google Scholar 

  10. Tehrani-Bagha AR, Mahmoodi NM, Menger FM (2010) Degradation of a persistent organic dye from colored textile wastewater by ozonation. Desalination 260(1–3):34–38

    Article  CAS  Google Scholar 

  11. Yao Y, Bing H, Feifei X, Xiaofeng C (2011) Equilibrium and kinetic studies of methyl orange adsorption on multiwalled carbon nanotubes. Chem Eng J 170(1):82–89

    Article  CAS  Google Scholar 

  12. Chang PR, Zheng P, Liu B, Anderson DP, Yu J, Ma X (2011) Characterization of magnetic soluble starch-functionalized carbon nanotubes and its application for the adsorption of the dyes. J Hazard Mater 186(2–3):2144–2150

    Article  CAS  Google Scholar 

  13. Eskandarian L, Arami M, Pajootan E (2014) Evaluation of adsorption characteristics of multiwalled carbon nanotubes modified by a poly(propylene imine) dendrimer in single and multiple dye solutions: isotherms, kinetics, and thermodynamics. J Chem Eng Data 59(2):444–454

    Article  CAS  Google Scholar 

  14. Zheng S, Guo H, Yang F, Hong B (2015) Novel organic dye sorbent: synthesis and adsorption properties of multi-walled carbon nanotubes modified with gallic amide units. Desalin Water Treat 57(26):12264–12273

    Article  CAS  Google Scholar 

  15. Ghobadi J, Arami M, Bahrami H, Mahmoodi NM (2013) Modification of carbon nanotubes with cationic surfactant and its application for removal of direct dyes. Desalin Water Treat 52(22–24):4356–4368

    Google Scholar 

  16. Wang S, Ng CW, Wang W, Li Q, Li L (2012) A comparative study on the adsorption of acid and reactive dyes on multiwall carbon nanotubes in single and binary dye systems. J Chem Eng Data 57(5):1563–1569

    Article  CAS  Google Scholar 

  17. Wu CH (2007) Studies of the equilibrium and thermodynamics of the adsorption of Cu2+ onto as-produced and modified carbon nanotubes. J Colloids Interface Sci 311(2):338–346

    Article  CAS  Google Scholar 

  18. Gong JL, Wang B, Zeng GM, Yang CP, Niu CG, Niu QY, Zhou WJ, Liang Y (2009) Removal of cationic dyes from aqueous solution using magnetic multi-wall carbon nanotube nanocomposite as adsorbent. J Hazard Mater 164(2–3):1517–1522

    Article  CAS  Google Scholar 

  19. Kierkowicz M, Pach E, Santidrián A, Sandoval S, Gonçalves G, Tobías-Rossell E, Kalbáč M, Ballesteros B, Tobias G (2018) Comparative study of shortening and cutting strategies of single-walled and multi-walled carbon nanotubes assessed by scanning electron microscopy. Carbon 139:922–932

    Article  CAS  Google Scholar 

  20. Park KC, Fujishige M, Takeuchi K, Arai S, Morimoto S, Endo M (2008) Inter-collisional cutting of multi-walled carbon nanotubes by high-speed agitation. J Phys Chem Solids 69(10):2481–2486

    Article  CAS  Google Scholar 

  21. Chiang Y-C, Lin W-H, Chang Y-C (2011) The influence of treatment duration on multi-walled carbon nanotubes functionalized by H2SO4/HNO3 oxidation. Appl Surf Sci 257(6):2401–2410

    Article  CAS  Google Scholar 

  22. Cheng J, Chang PR, Zheng P, Ma X (2014) Characterization of magnetic carbon nanotube–cyclodextrin composite and its adsorption of dye. Ind Eng Chem Res 53(4):1415–1421

    Article  CAS  Google Scholar 

  23. Hosseinzadeh S, Hosseinzadeh H, Pashaei S, Khodaparast Z (2018) Synthesis of magnetic functionalized MWCNT nanocomposite through surface RAFT co-polymerization of acrylic acid and N-isopropyl acrylamide for removal of cationic dyes from aqueous solutions. Ecotoxicol Environ Saf 161:34–44

    Article  CAS  Google Scholar 

  24. Gumus H (2018) Determination of progress in acrylic acid modification on polyvinylidene fluoride membrane by infrared spectroscopy. J Mol Struct 1174:122–126

    Article  CAS  Google Scholar 

  25. Liang S, Li G, Tian R (2015) Multi-walled carbon nanotubes functionalized with a ultrahigh fraction of carboxyl and hydroxyl groups by ultrasound-assisted oxidation. J Mater Sci 51(7):3513–3524. https://doi.org/10.1007/s10853-015-9671-z

    Article  CAS  Google Scholar 

  26. Zhao Z, Yang Z, Hu Y, Li J, Fan X (2013) Multiple functionalization of multi-walled carbon nanotubes with carboxyl and amino groups. Appl Surf Sci 276:476–481

    Article  CAS  Google Scholar 

  27. Shao D, Sheng G, Chen C, Wang X, Nagatsu M (2010) Removal of polychlorinated biphenyls from aqueous solutions using beta-cyclodextrin grafted multiwalled carbon nanotubes. Chemosphere 79(7):679–685

    Article  CAS  Google Scholar 

  28. Datsyuk V, Kalyva M, Papagelis K, Parthenios J, Tasis D, Siokou A, Kallitsis I, Galiotis C (2008) Chemical oxidation of multiwalled carbon nanotubes. Carbon 46(6):833–840

    Article  CAS  Google Scholar 

  29. He J, Shang H, Zhang X, Sun X (2018) Synthesis and application of ion imprinting polymer coated magnetic multi-walled carbon nanotubes for selective adsorption of nickel ion. Appl Surf Sci 428:110–117

    Article  CAS  Google Scholar 

  30. Martín O, Gutierrez HR, Maroto-Valiente A, Terrones M, Blanco T, Baselga J (2013) An efficient method for the carboxylation of few-wall carbon nanotubes with little damage to their sidewalls. Mater Chem Phys 140(2–3):499–507

    Article  CAS  Google Scholar 

  31. Mittal A, Mittal J, Malviya A, Kaur D, Gupta VK (2010) Adsorption of hazardous dye crystal violet from wastewater by waste materials. J Colloids Interface Sci 343(2):463–473

    Article  CAS  Google Scholar 

  32. Wu F-c, Tseng R-l, Juang R-s (2001) Kinetic modeling of liquid-phase adsorption of reactive dyes and metal ions on chitosan. Water Res 35(3):613–618

    Article  CAS  Google Scholar 

  33. Wang P, Cao M, Wang C, Ao Y, Hou J, Qian J (2014) Kinetics and thermodynamics of adsorption of methylene blue by a magnetic graphene–carbon nanotube composite. Appl Surf Sci 290:116–124

    Article  CAS  Google Scholar 

  34. Robati D, Mirza B, Ghazisaeidi R, Rajabi M, Moradi O, Tyagi I, Agarwal S, Gupta VK (2016) Adsorption behavior of methylene blue dye on nanocomposite multi-walled carbon nanotube functionalized thiol (MWCNT-SH) as new adsorbent. J Mol Liq 216:830–835

    Article  CAS  Google Scholar 

  35. Li Y, Du Q, Liu T, Peng X, Wang J, Sun J, Wang Y, Wu S, Wang Z, Xia Y, Xia L (2013) Comparative study of methylene blue dye adsorption onto activated carbon, graphene oxide, and carbon nanotubes. Chem Eng Res Des 91(2):361–368

    Article  CAS  Google Scholar 

  36. Ahamad T, Naushad M, Eldesoky GE, Al-Saeedi SI, Nafady A, Al-Kadhi NS, AaH Al-Muhtaseb, Khan AA, Khan A (2019) Effective and fast adsorptive removal of toxic cationic dye (MB) from aqueous medium using amino-functionalized magnetic multiwall carbon nanotubes. J Mol Liq 282:154–161

    Article  CAS  Google Scholar 

  37. Yan H, Tao X, Yang Z, Li K, Yang H, Li A, Cheng R (2014) Effects of the oxidation degree of graphene oxide on the adsorption of methylene blue. J Hazard Mater 268:191–198

    Article  CAS  Google Scholar 

  38. Yang K, Xing B (2010) Adsorption of organic compounds by carbon nanomaterials in aqueous phase: Polanyi theory and its application. Chem Rev 110:5989–6008

    Article  CAS  Google Scholar 

  39. Ghaffar A, Younis MN (2015) Interaction and thermodynamics of methylene blue adsorption on oxidized multi-walled carbon nanotubes. Green Process Synth 4(3):209–217

    CAS  Google Scholar 

  40. Yang K, Xing B (2009) Adsorption of fulvic acid by carbon nanotubes from water. Environ Pollut 157(4):1095–1100

    Article  CAS  Google Scholar 

  41. Hyung H, Kim J-h (2008) Natural organic matter (NOM) adsorption to multi-walled carbon nanotubes: effect of NOM characteristics and water quality parameters. Environ Sci Technol 42:4416–4421

    Article  CAS  Google Scholar 

  42. Franz M, Arafat HA, Pinto NG (2000) Effect of chemical surface heterogeneity on the adsorption mechanism of dissolved aromatics on activated carbon. Carbon 38:1807–1819

    Article  CAS  Google Scholar 

  43. Wu T, Cai X, Tan S, Li H, Liu J, Yang W (2011) Adsorption characteristics of acrylonitrile, p-toluenesulfonic acid, 1-naphthalenesulfonic acid and methyl blue on graphene in aqueous solutions. Chem Eng J 173(1):144–149

    Article  CAS  Google Scholar 

  44. Pan B, Xing B (2008) Adsorption mechanisms of organic chemicals on carbon nanotubes. Environ Sci Technol 42:9005–9012

    Article  CAS  Google Scholar 

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Acknowledgements

The work was supported by the National Natural Science Foundation of China (No. 51378350) and the Nature Science Foundation of Tianjin City (No. 17JCTPJC47000).

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Correspondence to Guangfen Li.

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Huan, Y., Wang, G., Li, C. et al. Acrylic acid grafted-multi-walled carbon nanotubes and their high-efficiency adsorption of methylene blue. J Mater Sci 55, 4656–4670 (2020). https://doi.org/10.1007/s10853-019-04167-3

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