journal article·2019-12Open access

Functionalized magnetic biopolymeric graphene oxide with outstanding performance in water purification

Amit Kumar Sarkar, John Kwame Bediako, Jong-Won Choi, Yeoung-Sang Yun

NPG Asia Materials· Volume 11· Issue 1

Abstract

Abstract Graphene oxide (GO) is an attractive material for water treatment, although its high surface energy restricts its practical application. To overcome this challenge, we have developed a well-dispersed and interconnected, functionalized biopolymeric GO with magnetic activity, namely, cl–CS–p(MA)/Fe3O4NPs. This three-dimensional, sponge-like nanostructured material is composed of graphene oxide nanosheets dispersed in functionalized chitosan/poly(methacrylic acid) and is cross-linked with in situ-developed Fe3O4 nanoparticles. Methacrylic acid (MA)-functionalized chitosan (CS) cross-linked with N,N-methylenebis(acrylamide) (MBA), designated as cl–CS–p(MA), facilitates the stable dispersion of GO nanosheets, providing a proper solid matrix for the generation of well-dispersed in situ Fe3O4NPs. The methodology allows for the generation of numerous binding sites with an interconnected morphology, facilitating the rapid uptake of a cationic dye in significant quantity, e.g., methylene blue (MB), which is used as a model water pollutant. In this work, the structural architecture of cl–CS–p(MA)/Fe3O4NPs was characterized with multiple approaches, and the adsorption mechanism was revealed to be an electrostatic interaction. The synthesized nanocomposite showed significant recyclability and structural stability. Adsorption equilibrium was achieved within 20 min, and the maximum adsorption capacity was 2478 mg/g for MB, surpassing the values reported for any other adsorbents to date.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Graphene and Nanomaterials Applications · Graphene research and applications · Adsorption and biosorption for pollutant removal

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (52)

Show source-provided references
1. Khin, M. M., Nair, A. S., Babu, V. J., Murugan, R. & Ramakrishna, S. A review on nanomaterials for environmental remediation. Energy & Environ. Sci. 5, 8075–8109 (2012).10.1039/c2ee21818f ↗
2. Cheng, H. N., Doemeny, L. J., Geraci, C. L. & Grob Schmidt, D. Nanotechnology Overview: Opportunities and Challenges in Nanotechnology: Delivering on the Promise Vol 1, (eds. Cheng, H. N., Doemeny, L. J., Geraci, C. L. & Grob Schmidt, D.) Ch. 1, 1–12 (American Chemical Society, USA, 2016).
3. Nardecchia, S., Carriazo, D., Ferrer, M. L., Gutierrez, M. C. & del Monte, F. Three dimensional macroporous architectures and aerogels built of carbon nanotubes and/or graphene: synthesis and applications. Chem. Soc. Rev. 42, 794–830 (2013).10.1039/C2CS35353A ↗
4. Dongyun, C. et al. Micro–nanocomposites in environmental management. Adv. Mater. 28, 10443–10458 (2016).10.1002/adma.201601486 ↗
5. Byun, J., Patel, H. A., Thirion, D. & Yavuz, C. T. Charge-specific size-dependent separation of water-soluble organic molecules by fluorinated nanoporous networks. Nat. Commun. 7, 13377 (2016).10.1038/ncomms13377 ↗
6. Aguila, B. et al. Efficient mercury capture using functionalized porous organic polymer. Advanced Materials 29, 1–6 (2017).10.1002/adma.201700665 ↗
7. Hameed, B. H., Din, A. T. M. & Ahmad, A. L. Adsorption of methylene blue onto bamboo-based activated carbon: Kinetics and equilibrium studies. J. Hazard. Mater. 141, 819–825 (2007).10.1016/j.jhazmat.2006.07.049 ↗
8. Wang, S. & Peng, Y. Natural zeolites as effective adsorbents in water and wastewater treatment. Chem. Eng. J. 156, 11–24 (2010).10.1016/j.cej.2009.10.029 ↗
9. Peng, N. et al. Superabsorbentcellulose–clay nanocomposite hydrogels for highly efficient removal of dye in water. ACS Sustain. Chem. & Eng. 4, 7217–7224 (2016).10.1021/acssuschemeng.6b02178 ↗
10. Sarkar, A. K., Saha, A., Panda, A. B. & Pal, S. pH Triggered superior selective adsorption and separation of both cationic and anionic dyes and photocatalytic activity on a fully exfoliated titanate layer-natural polymer based nanocomposite. Chem. Commun. 51, 16057–16060 (2015).10.1039/C5CC06214D ↗
11. Zhuang, X., Wan, Y., Feng, C., Shen, Y. & Zhao, D. Highly efficient adsorption of bulky dye molecules in wastewater on ordered mesoporous carbons. Chem. Mater. 21, 706–716 (2009).10.1021/cm8028577 ↗
12. Homaeigohar, S., Zillohu, A., Abdelaziz, R., Hedayati, M. & Elbahri, M. A novel nanohybrid nanofibrous adsorbent for water purification from dye pollutants. Materials 9, 848 (2016).10.3390/ma9100848 ↗
13. Shahin, H., Thomas, S., Julian, S., Lorenz, K. & Mady, E. A flexible oxygenated carbographite nanofilamentous buckypaper as an amphiphilic membrane. Adv. Mater. Interfaces 5, 1800001 (2018).10.1002/admi.201800001 ↗
14. Janaki, V. et al. Polyaniline/chitosan composite: an eco-friendly polymer for enhanced removal of dyes from aqueous solution. Synth. Met. 162, 974–980 (2012).10.1016/j.synthmet.2012.04.015 ↗
15. Compton, O. C. & Nguyen, S. T. Graphene oxide, highly reduced graphene oxide, and graphene: versatile building blocks for carbon-based materials. Small 6, 711–723 (2010).10.1002/smll.200901934 ↗
16. Yan, H. et al. Influence of the surface structure of graphene oxide on the adsorption of aromatic organic compounds from water. ACS Appl. Mater. & Interfaces 7, 6690–6697 (2015).10.1021/acsami.5b00053 ↗
17. Liu, F., Chung, S., Oh, G. & Seo, T. S. Three-dimensional graphene oxide nanostructure for fast and efficient water-soluble dye removal. ACS Appl. Mater. & Interfaces 4, 922–927 (2012).10.1021/am201590z ↗
18. Zhang, J. et al. Poly(acrylic acid) functionalized magnetic graphene oxide nanocomposite for removal of methylene blue. RSC Adv. 5, 32272–32282 (2015).10.1039/C5RA01815C ↗
19. Cheng, Z. et al. One-step fabrication of graphene oxide enhanced magnetic composite gel for highly efficient dye adsorption and catalysis. ACS Sustain. Chem. & Eng. 3, 1677–1685 (2015).10.1021/acssuschemeng.5b00383 ↗
20. Bi, H. et al. Highly enhanced performance of spongy graphene as an oil sorbent. J. Mater. Chem. A 2, 1652–1656 (2014).10.1039/C3TA14112H ↗
21. Bao, C. et al. Graphene oxide beads for fast clean-up of hazardous chemicals. J. Mater. Chem. A 4, 9437–9446 (2016).10.1039/C6TA01411A ↗
22. Yang, Y. et al. Preparation of reduced graphene oxide/poly(acrylamide) nanocomposite and Its Adsorption of Pb(II) and methylene blue. Langmuir 29, 10727–10736 (2013).10.1021/la401940z ↗
23. Yu, R. et al. Graphene oxide/chitosan aerogel microspheres with honeycomb-cobweb and radially oriented microchannel structures for broad-spectrum and rapid adsorption of water contaminants. ACS Appl. Mater. & Interfaces 9, 21809–21819 (2017).10.1021/acsami.7b04655 ↗
24. Morrow, B. H., Payne, G. F. & Shen, J. pH-Responsive self-assembly of polysaccharide through a rugged energy landscape. J. Am. Chem. Soc. 137, 13024–13030 (2015).10.1021/jacs.5b07761 ↗
25. Hummers, W. S. & Offeman, R. E. Preparation of graphitic oxide. J. Am. Chem. Soc. 80, 1339–1339 (1958).10.1021/ja01539a017 ↗
26. Marcano, D. C. et al. Improved synthesis of graphene oxide. ACS Nano 4, 4806–4814 (2010).10.1021/nn1006368 ↗
27. Liu, Q., Zhong, L.-B., Zhao, Q.-B., Frear, C. & Zheng, Y.-M. Synthesis of Fe3O4/Polyacrylonitrile Composite electrospun nanofiber mat for effective adsorption of tetracycline. ACS Appl. Mater. & Interfaces 7, 14573–14583 (2015).10.1021/acsami.5b04598 ↗
28. Xu, X. et al. Self-sensing, ultralight, and conductive 3D graphene/iron oxide aerogel elastomer deformable in a magnetic field. ACS Nano 9, 3969–3977 (2015).10.1021/nn507426u ↗
29. Mondal, A., Maiti, S., Singha, K., Mahanty, S. & Panda, A. B. TiO2-rGO nanocomposite hollow spheres: large scale synthesis and application as an efficient anode material for lithium-ion batteries. J. Mater. Chem. A 5, 23853–23862 (2017).10.1039/C7TA08164B ↗
30. Yang, X., Tu, Y., Li, L. & Shang, S. & Tao X.m. Well-dispersed chitosan/graphene oxide nanocomposites. ACS Appl. Mater. & Interfaces 2, 1707–1713 (2010).10.1021/am100222m ↗
31. Zhan, Y. et al. Cross-linkable nitrile functionalized graphene oxide/poly(arylene ether nitrile) nanocomposite films with high mechanical strength and thermal stability. J. Mater. Chem. 22, 5602–5608 (2012).10.1039/c2jm15780b ↗
32. Darder, M., Colilla, M. & Ruiz-Hitzky, E. Biopolymer−clay nanocomposites based on chitosan intercalated in montmorillonite. Chem. Mater. 15, 3774–3780 (2003).10.1021/cm0343047 ↗
33. Woo, H. et al. Facile synthesis of hybrid Cu2O/Pd-Fe3O4 nanocatalysts for C-H arylation of 4-nitroimidazoles. RSC Adv. 6, 36211–36217 (2016).10.1039/C6RA05068A ↗
34. Lopez-Perez, P. M., Marques, A. P., Silva, R. M. Pd, Pashkuleva, I. & Reis, R. L. Effect of chitosan membrane surface modification via plasma induced polymerization on the adhesion of osteoblast-like cells. J. Mater. Chem. 17, 4064–4071 (2007).10.1039/b707326g ↗
35. Fujii, T. et al. In situ. Phys. Rev. B 59, 3195–3202 (1999).10.1103/PhysRevB.59.3195 ↗
36. Bo, Z. et al. Green preparation of reduced graphene oxide for sensing and energy storage applications. Sci. Rep. 4, 4684 (2014).
37. Chang, Y. et al. Synthesis of 3D nitrogen-doped graphene/Fe3O4 by a metal ion induced self-assembly process for high-performance Li-ion batteries. J. Mater. Chem. A 1, 14658–14665 (2013).10.1039/c3ta13370b ↗
38. Le, X. T., Doan, N. D., Dequivre, T., Viel, P. & Palacin, S. Covalent grafting of chitosan onto stainless steel through aryldiazonium self-adhesive layers. ACS Appl. Mater. & Interfaces 6, 9085–9092 (2014).10.1021/am500582e ↗
39. Lu, Y.-F. et al. Nitrogen-doped graphene sheets grown by chemical vapor deposition: synthesis and influence of nitrogen impurities on carrier transport. ACS Nano 7, 6522–6532 (2013).10.1021/nn402102y ↗
40. Sarkar, A. K., Pal, A., Ghorai, S., Mandre, N. R. & Pal, S. Efficient removal of malachite green dye using biodegradable graft copolymer derived from amylopectin and poly(acrylic acid). Carbohydr. Polym. 111, 108–115 (2014).10.1016/j.carbpol.2014.04.042 ↗
41. Langmuir, I. The adsorption of gases on plane surfaces of glass, mica and platinum. J. Am. Chem. Soc. 40, 1361–1403 (1918).10.1021/ja02242a004 ↗
42. Freundlich, H. M. F. Over the adsorption in solution. J. Phys. Chem. 57, 385–471 (1906).
43. Sips, R. On the structure of a catalyst surface. J. Chem. Phys. 16, 490–495 (1948).10.1063/1.1746922 ↗
44. Vargas, A. M. M., Cazetta, A. L., Kunita, M. H., Silva, T. L. & Almeida, V. C. Adsorption of methylene blue on activated carbon produced from flamboyant pods (Delonix regia): Study of adsorption isotherms and kinetic models. Chem. Eng. J. 168, 722–730 (2011).10.1016/j.cej.2011.01.067 ↗
45. Dolatkhah, A. & Wilson, L. D. Magnetite/polymer brush nanocomposites with switchable uptake behavior toward methylene blue. ACS Appl. Mater. & Interfaces 8, 5595–5607 (2016).10.1021/acsami.5b11599 ↗
46. Hu, L. et al. Fabrication of magnetic water-soluble hyperbranched polyol functionalized graphene oxide for high-efficiency water remediation. Sci. Rep. 6, 28924 (2016).
47. Haque, E., Lo, V., Minett, A. I., Harris, A. T. & Church, T. L. Dichotomous adsorption behaviour of dyes on an amino-functionalised metal-organic framework, amino-MIL-101(Al). J. Mater. Chem. A 2, 193–203 (2014).10.1039/C3TA13589F ↗
48. Huang, L., He, M., Chen, B., Cheng, Q. & Hu, B. Facile green synthesis of magnetic porous organic polymers for rapid removal and separation of methylene blue. ACS Sustain. Chem. & Eng. 5, 4050–4055 (2017).10.1021/acssuschemeng.7b00031 ↗
49. Chen, D., Wang, L., Ma, Y. & Yang, W. Super-adsorbent material based on functional polymer particles with a multilevel porous structure. Npg Asia Mater. 8, e301 (2016).10.1038/am.2016.117 ↗
50. Lagergren, S. About the theory of so-called adsorption of soluble substances. Handlingar 24, 1–39 (1898).
51. Ho, Y.-S. Second-order kinetic model for the sorption of cadmium onto tree fern: A comparison of linear and non-linear methods. Water Res. 40, 119–125 (2006).10.1016/j.watres.2005.10.040 ↗
52. Ito, Y., Cong, W., Fujita, T., Tang, Z. & Chen, M. High catalytic activity of nitrogen and sulfur Co-doped nanoporous graphene in the hydrogen evolution reaction. Angew. Chem. Int. Ed. 54, 2131–2136 (2015).10.1002/anie.201410050 ↗