Abstract
The graphene based materials in water pollutant treatment have recently gained significant attention due to their high surface area, high mechanical strength and tuneable surface chemistry. However, the relatively high cost, poor hydrophobicity, low adsorption capacity, and recyclability limit their practical application. Here in, driven by need, we report a simple approach for the synthesis of graphene quantum dots (GQDs) via pyrolysis, preferred because of high controllability and fewer defects over chemical exfoliation methods. The synthesized GQDs are further embedded on bacterial cellulose nanopaper (BCN) and characterized using spectroscopy and microscopy techniques. Furthermore, the well-ordered multi-layered GQD embedded BCN based filtration assembly is designed and developed for treatment of water pollutants and industrial dye wastewater. The multi-layered GQD embedded BCN based filtration assembly is validated by purifying industrial dye and heavy metal (Hg2+, Pb2+) with removal efficiency of 99.6% and 97%, respectively. Our multi-layered filtration assembly demonstrated significant membrane regeneration capacity until six cycles. The isotherm model also showed an appropriate fit exhibiting good adsorption behaviour. Our multi-layered filtration assembly can be established as a promising filtration assembly for inexpensive, efficient and low energy applications in wastewater treatment.
Graphic abstract
Similar content being viewed by others
References
Almasian A, Giahi M, Chizari Fard Gh et al (2018) Removal of heavy metal ions by modified PAN/PANI-nylon core-shell nanofibers membrane: filtration performance, antifouling and regeneration behavior. Chem Eng J 351:1166–1178. https://doi.org/10.1016/j.cej.2018.06.127
Awadallah-F A (2017) Adsorptive removal of malachite green chloride and reactive red-198 from aqueous solutions by using multiwall carbon nanotubes-graft-poly (2-acrylamido-2-methyl-1-propanesulfonic acid). J Polym Environ 25:258–276. https://doi.org/10.1007/s10924-016-0804-5
Bacon M, Bradley SJ, Nann T (2014) Graphene quantum dots. Part Part Syst Charact 31:415–428. https://doi.org/10.1002/ppsc.201300252
Baker SN, Baker GA (2010) Luminescent carbon nanodots: emergent nanolights. Angew Chem Int Ed 49:6726–6744. https://doi.org/10.1002/anie.200906623
Bal A, Özkahraman B, Acar I et al (2014) Study on adsorption, regeneration, and reuse of crosslinked chitosan graft copolymers for Cu(II) ion removal from aqueous solutions. Desalin Water Treat 52:3246–3255. https://doi.org/10.1080/19443994.2013.800276
Bi R, Zhang R, Shen J et al (2019) Graphene quantum dots engineered nanofiltration membrane for ultrafast molecular separation. J Membr Sci 572:504–511. https://doi.org/10.1016/j.memsci.2018.11.044
Chen H, Wang A (2009) Adsorption characteristics of Cu(II) from aqueous solution onto poly(acrylamide)/attapulgite composite. J Hazard Mater 165:223–231. https://doi.org/10.1016/j.jhazmat.2008.09.097
Chua CK, Sofer Z, Šimek P et al (2015) Synthesis of strongly fluorescent graphene quantum dots by cage-opening buckminsterfullerene. ACS Nano 9:2548–2555. https://doi.org/10.1021/nn505639q
Cui J, Li F, Wang Y et al (2020) Electrospun nanofiber membrane for wastewater treatment applications. Sep Purif Technol 250:117116. https://doi.org/10.1016/j.seppur.2020.117116
Dong Y, Li G, Zhou N et al (2012a) Graphene quantum dot as a green and facile sensor for free chlorine in drinking water. Anal Chem 84:8378–8382. https://doi.org/10.1021/ac301945z
Dong Y, Shao J, Chen C et al (2012b) Blue luminescent graphene quantum dots and graphene oxide prepared by tuning the carbonization degree of citric acid. Carbon 50:4738–4743. https://doi.org/10.1016/j.carbon.2012.06.002
Donkadokula NY, Kola AK, Naz I, Saroj D (2020) A review on advanced physico-chemical and biological textile dye wastewater treatment techniques. Rev Environ Sci Biotechnol 19:543–560. https://doi.org/10.1007/s11157-020-09543-z
Eda G, Lin Y-Y, Mattevi C et al (2010) Blue photoluminescence from chemically derived graphene oxide. Adv Mater 22:505–509. https://doi.org/10.1002/adma.200901996
French AD (2017) Glucose, not cellobiose, is the repeating unit of cellulose and why that is important. Cellulose 24:4605–4609. https://doi.org/10.1007/s10570-017-1450-3
Haque E, Kim J, Malgras V et al (2018) Recent advances in graphene quantum dots: synthesis, properties, and applications. Small Methods 2:1800050. https://doi.org/10.1002/smtd.201800050
Herington AC, Ymer SI, Stevenson JL (1986) Affinity purification and structural characterization of a specific binding protein for human growth hormone in human serum. Biochem Biophys Res Commun 139:150–155. https://doi.org/10.1016/s0006-291x(86)80092-4
Jiang F, Chen D, Li R et al (2013) Eco-friendly synthesis of size-controllable amine-functionalized graphene quantum dots with antimycoplasma properties. Nanoscale 5:1137. https://doi.org/10.1039/c2nr33191h
Ju S-Y, Kopcha WP, Papadimitrakopoulos F (2009) Brightly fluorescent single-walled carbon nanotubes via an oxygen-excluding surfactant organization. Science 323:1319–1323. https://doi.org/10.1126/science.1166265
Kalluri A, Debnath D, Dharmadhikari B, Patra P (2018) Graphene Quantum Dots: Synthesis and Applications. In: Methods in Enzymology. Elsevier, pp 335–354
Kanth N, Xu W, Prasad U et al (2020) PMMA-TiO2 fibers for the photocatalytic degradation of water pollutants. Nanomaterials 10:1279. https://doi.org/10.3390/nano10071279
Kong L, Xiong Y, Sun L et al (2014) Sorption performance and mechanism of a sludge-derived char as porous carbon-based hybrid adsorbent for benzene derivatives in aqueous solution. J Hazard Mater 274:205–211. https://doi.org/10.1016/j.jhazmat.2014.04.014
Kumawat MK, Thakur M, Gurung RB, Srivastava R (2017) Graphene quantum dots from Mangifera indica: application in near-infrared bioimaging and intracellular nanothermometry. ACS Sustainable Chem Eng 5:1382–1391. https://doi.org/10.1021/acssuschemeng.6b01893
Li X, Wang X, Zhang L et al (2008) Chemically derived, ultrasmooth graphene nanoribbon semiconductors. Science 319:1229–1232. https://doi.org/10.1126/science.1150878
Li Q, Chen B, Xing B (2017) Aggregation kinetics and self-assembly mechanisms of graphene quantum dots in aqueous solutions: cooperative effects of pH and electrolytes. Environ Sci Technol 51:1364–1376. https://doi.org/10.1021/acs.est.6b04178
Liu F, Wang L, Li D et al (2020a) Preparation and characterization of novel thin film composite nanofiltration membrane with PVDF tree-like nanofiber membrane as composite scaffold. Mater Des 196:109101. https://doi.org/10.1016/j.matdes.2020.109101
Liu Q, Sun J, Gao K et al (2020b) Graphene quantum dots for energy storage and conversion: from fabrication to applications. Mater Chem Front 4:421–436. https://doi.org/10.1039/C9QM00553F
Loh KP, Bao Q, Eda G, Chhowalla M (2010) Graphene oxide as a chemically tunable platform for optical applications. Nature Chem 2:1015–1024. https://doi.org/10.1038/nchem.907
Mansuriya B, Altintas Z (2020) Applications of graphene quantum dots in biomedical sensors. Sensors 20:1072. https://doi.org/10.3390/s20041072
Minati DP (2019) Facile synthesis of water-soluble, highly-fluorescent graphene quantum dots from graphene oxide reduction for efficient cell labelling. J Carbon Res. https://doi.org/10.3390/c5040077
Nair AK, JagadeeshBabu PE (2017) Ag-TiO2 nanosheet embedded photocatalytic membrane for solar water treatment. J Environ Chem Eng 5:4128–4133. https://doi.org/10.1016/j.jece.2017.07.046
Nie S, Hao N, Zhang K et al (2020) Cellulose nanofibrils-based thermally conductive composites for flexible electronics: a mini review. Cellulose 27:4173–4187. https://doi.org/10.1007/s10570-020-03103-y
Pasini SM, Valério A, Yin G et al (2021) An overview on nanostructured TiO2–containing fibers for photocatalytic degradation of organic pollutants in wastewater treatment. J Water Process Eng 40:101827. https://doi.org/10.1016/j.jwpe.2020.101827
Selvaraj V, Swarna Karthika T, Mansiya C, Alagar M (2021) An over review on recently developed techniques, mechanisms and intermediate involved in the advanced azo dye degradation for industrial applications. J Mol Struct 1224:129195. https://doi.org/10.1016/j.molstruc.2020.129195
Shaker MA, Yakout AA (2016) Optimization, isotherm, kinetic and thermodynamic studies of Pb(II) ions adsorption onto N-maleated chitosan-immobilized TiO 2 nanoparticles from aqueous media. Spectrochim Acta Part A Mol Biomol Spectrosc 154:145–156. https://doi.org/10.1016/j.saa.2015.10.027
Shindhal T, Rakholiya P, Varjani S et al (2021) A critical review on advances in the practices and perspectives for the treatment of dye industry wastewater. Bioengineered 12:70–87. https://doi.org/10.1080/21655979.2020.1863034
Sjahro N, Yunus R, Abdullah LC et al (2021) Recent advances in the application of cellulose derivatives for removal of contaminants from aquatic environments. Cellulose. https://doi.org/10.1007/s10570-021-03985-6
Song SH, Jang M-H, Chung J et al (2014a) Graphene: highly efficient light-emitting diode of graphene quantum dots fabricated from graphite intercalation compounds (advanced optical materials 11/2014). Adv Op Mater 2:1009–1009. https://doi.org/10.1002/adom.201470066
Song SH, Jang M-H, Chung J et al (2014b) Highly efficient light-emitting diode of graphene quantum dots fabricated from graphite intercalation compounds. Adv Op Mater 2:1016–1023. https://doi.org/10.1002/adom.201400184
Song S-H, Jang M, Yoon H et al (2016) Size and pH dependent photoluminescence of graphene quantum dots with low oxygen content. RSC Adv 6:97990–97994. https://doi.org/10.1039/C6RA21651J
Sun H, Wu L, Wei W, Qu X (2013) Recent advances in graphene quantum dots for sensing. Mater Today 16:433–442. https://doi.org/10.1016/j.mattod.2013.10.020
Vatanpour V, Mousavi Khadem SS, Masteri-Farahani M et al (2020) Anti-fouling and permeable polyvinyl chloride nanofiltration membrane embedded by hydrophilic graphene quantum dots for dye wastewater treatment. J Water Process Eng 38:101652. https://doi.org/10.1016/j.jwpe.2020.101652
Wang L, Wang Y, Xu T et al (2014) Gram-scale synthesis of single-crystalline graphene quantum dots with superior optical properties. Nat Commun 5:5357. https://doi.org/10.1038/ncomms6357
Wu X, Si Y, Yu J, Ding B (2018) Titania-based electrospun nanofibrous materials: a new model for organic pollutants degradation. MRS Commun 8:765–781. https://doi.org/10.1557/mrc.2018.139
Xu X, Ray R, Gu Y et al (2004) Electrophoretic analysis and purification of fluorescent single-walled carbon nanotube fragments. J Am Chem Soc 126:12736–12737. https://doi.org/10.1021/ja040082h
Xue J, Wu T, Dai Y, Xia Y (2019) Electrospinning and electrospun nanofibers: methods, materials, and applications. Chem Rev 119:5298–5415. https://doi.org/10.1021/acs.chemrev.8b00593
Xue J, Shen J, Zhang R et al (2020) High-flux nanofiltration membrane prepared with β-cyclodextrin and graphene quantum dots. J Membr Sci 612:118465. https://doi.org/10.1016/j.memsci.2020.118465
Yan X, Cui X, Li L (2010) Synthesis of large, stable colloidal graphene quantum dots with tunable size. J Am Chem Soc 132:5944–5945. https://doi.org/10.1021/ja1009376
Yu S-J, Kang M-W, Chang H-C et al (2005) Bright fluorescent nanodiamonds: no photobleaching and low cytotoxicity. J Am Chem Soc 127:17604–17605. https://doi.org/10.1021/ja0567081
Yuan A, Lei H, Xi F et al (2019) Graphene quantum dots decorated graphitic carbon nitride nanorods for photocatalytic removal of antibiotics. J Colloid Interface Sci 548:56–65
Acknowledgments
We gratefully acknowledge Department of Science and Technology, Govt of India (DST/TMD(EWO)/OWUIS-2018/RS-20(G)) for financial support.
Dr Gajendra Singh Vishwakarma gratefully acknowledge GSBTM, Govt of Gujarat, India (GSBTM/JDR&D/604-2019/307) for financial support. We acknowledge Mr. Ravindrasinh Rehewar, CEO, SVA Robotics, India for the support of product design and development.
Author information
Authors and Affiliations
Corresponding authors
Ethics declarations
Conflict of interest
The authors declare that we do not have any conflict of interest in submission of this manuscript.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Pandya, A., Shah, K., Prajapati, H. et al. GQD embedded bacterial cellulose nanopaper based multi-layered filtration membranes assembly for industrial dye and heavy metal removal in wastewater. Cellulose 28, 10385–10398 (2021). https://doi.org/10.1007/s10570-021-04174-1
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10570-021-04174-1