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.
This is a preview of subscription content, log in to check access.
Buy single article
Instant unlimited access to the full article PDF.
Price includes VAT for USA
Subscribe to journal
Immediate online access to all issues from 2019. Subscription will auto renew annually.
This is the net price. Taxes to be calculated in checkout.
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
Wu CH (2007) Adsorption of reactive dye onto carbon nanotubes: equilibrium, kinetics and thermodynamics. J Hazard Mater 144(1–2):93–100
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
Gumus H (2018) Determination of progress in acrylic acid modification on polyvinylidene fluoride membrane by infrared spectroscopy. J Mol Struct 1174:122–126
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
Yang K, Xing B (2009) Adsorption of fulvic acid by carbon nanotubes from water. Environ Pollut 157(4):1095–1100
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
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
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
Pan B, Xing B (2008) Adsorption mechanisms of organic chemicals on carbon nanotubes. Environ Sci Technol 42:9005–9012
The work was supported by the National Natural Science Foundation of China (No. 51378350) and the Nature Science Foundation of Tianjin City (No. 17JCTPJC47000).
Conflict of interest
The authors declare that they have no conflict of interests.
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
About this article
Cite this article
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