Skip to main content
Log in

Glutaraldehyde and polyvinyl alcohol crosslinked cellulose membranes for efficient methyl orange and Congo red removal

  • Original Research
  • Published:
Cellulose Aims and scope Submit manuscript

Abstract

Self-standing and flexible regenerated cellulose membranes were fabricated by using a facile ZnCl2/CaCl2/cellulose dissolution system. The filtration experiments of the membranes were conducted by using methyl orange and Congo red as water contaminations. To improve the selectivity and stability, the crosslinkers of glutaraldehyde and polyvinyl alcohol were introduced to the membrane network. The best performance was observed over glutaraldehyde and polyvinyl alcohol crosslinked cellulose (P-G-RC) membrane with a Congo red rejection rate of 99.9% and a methyl orange rejection rate of 93.5%. The suitable pore radius (0.67 nm), low root-mean-square roughness (2.9 nm) and abundant hydroxyl groups were considered as the primary reasons contributed to the separation behavior. Furthermore, the P-G-RC membrane displayed excellent stability and reusability during the filtration tests.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Subscribe and save

Springer+
from $39.99 /Month
  • Starting from 10 chapters or articles per month
  • Access and download chapters and articles from more than 300k books and 2,500 journals
  • Cancel anytime
View plans

Buy Now

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7

Similar content being viewed by others

Explore related subjects

Discover the latest articles and news from researchers in related subjects, suggested using machine learning.

References

  • Bian H, Wei L, Lin C, Ma Q, Dai H, Zhu JY (2018) Lignin-containing cellulose nanofibril-reinforced polyvinyl alcohol hydrogels. ACS Sustain Chem Eng 6:4821–4828

    Article  CAS  Google Scholar 

  • Cai Q, Fan Z, Chen J, Guo W, Ma F, Sun S, Hu L, Zhou Q (2018) Dissolving process of bamboo powder analyzed by FT-IR spectroscopy. J Mol Struct 1171:639–643

    Article  CAS  Google Scholar 

  • Chen Y, He C (2017) High salt permeation nanofiltration membranes based on NMG-assisted polydopamine coating for dye/salt fractionation. Desalination 413:29–39

    Article  CAS  Google Scholar 

  • Chen W, Yu H, Lee SY, Wei T, Li J, Fan Z (2018) Nanocellulose: a promising nanomaterial for advanced electrochemical energy storage. Chem Soc Rev 47:2837–2872

    Article  CAS  PubMed  Google Scholar 

  • Feng Y, Wang Y, Liu S, Qiu J, Yao J (2017) Facile fabrication of ZIF-8 embedded millimeter-sized porous polyethersulfone beads for selective dye removal. Polym Compos 39:3896–3902

    Article  CAS  Google Scholar 

  • French AD (2014) Idealized powder diffraction patterns for cellulose polymorphs. Cellulose 21:885–896

    Article  CAS  Google Scholar 

  • Gu J, Hu C, Zhang W, Dichiara AB (2018) Reagentless preparation of shape memory cellulose nanofibril aerogels decorated with Pd nanoparticles and their application in dye discoloration. Appl Catal B Environ 237:482–490

    Article  CAS  Google Scholar 

  • Guo B, Chen W, Yan L (2013) Preparation of flexible, highly transparent, cross-linked cellulose thin film with high mechanical strength and low coefficient of thermal expansion. ACS Sustain Chem Eng 1:1474–1479

    Article  CAS  Google Scholar 

  • Gupta KM, Jiang J (2015) Cellulose dissolution and regeneration in ionic liquids: a computational perspective. Chem Eng Sci 121:180–189

    Article  CAS  Google Scholar 

  • Hamid NAA, Ismail AF, Matsuura T, Zularisam AW, Lau WJ, Yuliwati E, Abdullah MS (2011) Morphological and separation performance study of polysulfone/titanium dioxide (PSF/TiO2) ultrafiltration membranes for humic acid removal. Desalination 273:85–92

    Article  CAS  Google Scholar 

  • Hu M, Hu T, Li Z, Yang Y, Cheng R, Yang J, Cui C, Wang X (2018) Surface functional groups and interlayer water determine the electrochemical capacitance of Ti3C2Tx MXene. ACS Nano 12:3578–3586

    Article  CAS  PubMed  Google Scholar 

  • Huang J, Zhu H, Chen Y, Preston C, Rohrbach K, Cumings J, Hu L (2013) Highly transparent and flexible nanopaper transistors. ACS Nano 7:2106–2113

    Article  CAS  PubMed  Google Scholar 

  • Khalili MS, Zare K, Moradi O, Sillanpää M (2018) Preparation and characterization of MWCNT-COOH-cellulose-MgO NP nanocomposite as adsorbent for removal of methylene blue from aqueous solutions: isotherm, thermodynamic and kinetic studies. J Nanostruct Chem 8:103–121

    Article  CAS  Google Scholar 

  • Khoshsang H, Ghaffarinejad A, Kazemi H, Wang Y, Arandiyan H (2018) One-pot synthesis of S-doped Fe2O3/C magnetic nanocomposite as an adsorbent for anionic dye removal: equilibrium and kinetic studies. J Nanostruct Chem 8:23–32

    Article  CAS  Google Scholar 

  • Koli PB, Kapadnis KH, Deshpande UG, Patil MR (2018) Fabrication and characterization of pure and modified Co3O4 nanocatalyst and their application for photocatalytic degradation of eosine blue dye: a comparative study. J Nanostruct Chem 8:453–463

    Article  CAS  Google Scholar 

  • Kong L, Zhang D, Shao Z, Han B, Lv Y, Gao K, Peng X (2014) Superior effect of TEMPO-oxidized cellulose nanofibrils (TOCNs) on the performance of cellulose triacetate (CTA) ultrafiltration membrane. Desalination 332:117–125

    Article  CAS  Google Scholar 

  • Lin Q, Gao M, Chang J, Ma H (2017) Highly effective adsorption performance of carboxymethyl cellulose microspheres crosslinked with epichlorohydrin. J Appl Polym Sci 134:44363–44369

    Google Scholar 

  • Luo H, Dong J, Yao F, Yang Z, Li W, Wang J, Xu X, Hu J, Wan Y (2018) Layer-by-layer assembled bacterial cellulose/graphene oxide hydrogels with extremely enhanced mechanical properties. Nano Micro Lett 10:52–61

    Article  CAS  Google Scholar 

  • Lv Y, Du Y, Chen ZX, Qiu WZ, Xu ZK (2018) Nanocomposite membranes of polydopamine/electropositive nanoparticles/polyethyleneimine for nanofiltration. J Membr Sci 545:99–106

    Article  CAS  Google Scholar 

  • Moon RJ, Martini A, Nairn J, Simonsen J, Youngblood J (2011) Cellulose nanomaterials review: structure, properties and nanocomposites. Chem Soc Rev 40:3941–3994

    Article  CAS  PubMed  Google Scholar 

  • Ning R, Wu CN, Takeuchi M, Saito T, Isogai A (2017) Preparation and characterization of zinc oxide/TEMPO-oxidized cellulose nanofibril composite films. Cellulose 24:4861–4870

    Article  CAS  Google Scholar 

  • Pan Y, Shi X, Cai P, Guo T, Tong Z, Xiao H (2018) Dye removal from single and binary systems using gel-like bioadsorbent based on functional-modified cellulose. Cellulose 25:2559–2575

    Article  CAS  Google Scholar 

  • Park J, Oh M (2017) Construction of flexible metal-organic framework (MOF) papers through MOF growth on filter paper and their selective dye capture. Nanoscale 9:12850–12854

    Article  CAS  PubMed  Google Scholar 

  • Puspasari T, Pradeep N, Peinemann KV (2015) Crosslinked cellulose thin film composite nanofiltration membranes with zero salt rejection. J Membr Sci 491:132–137

    Article  CAS  Google Scholar 

  • Puspasari T, Huang T, Sutisna B, Peinemann KV (2018) Cellulose-polyethyleneimine blend membranes with anomalous nanofiltration performance. J Membr Sci 564:97–105

    Article  CAS  Google Scholar 

  • Robati D, Mirza B, Ghazisaeidi R, Rajabi M, Moradie O, Agarwalg S, Gupta VK (2016a) 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 

  • Robati D, Rajabi M, Moradi O, Najafi F, Tyagi I, Agarwal S, Gupta VK (2016b) Kinetics and thermodynamics of malachite green dye adsorption from aqueous solutions on graphene oxide and reduced graphene oxide. J Mol Liq 216:259–263

    Article  CAS  Google Scholar 

  • Robati D, Mirza B, Rajabi M, Moradi O, Tyagi I, Agarwal S, Gupta VK (2016c) Removal of hazardous Dyes-BR 12 and methyl orange using graphene oxide as an adsorbent from aqueous phase. Chem Eng J 284:687–697

    Article  CAS  Google Scholar 

  • Shen L, Yang Y, Zhao J, Wang X (2016) High-performance nanofiltration membrane prepared by dopamine-assisted interfacial polymerization on PES nanofibrous scaffolds. Desalin Water Treat 57:9549–9557

    Article  CAS  Google Scholar 

  • Sirus Z, Zinatizadeh AA, Rahimi M, Vatanpour V, Zangeneh H (2014) Preparation of a novel antifouling mixed matrix PES membrane by embedding graphene oxide nanoplates. J Membr Sci 453:292–301

    Article  CAS  Google Scholar 

  • Štefelová J, Slovák V, Siqueira G, Olsson RT, Tingaut P, Zimmermann T, Sehaqui H (2017) Drying and pyrolysis of cellulose nanofibers from wood, bacteria, and algae for char application in oil absorption and dye adsorption. ACS Sustain Chem Eng 5:2679–2692

    Article  CAS  Google Scholar 

  • Tanaka A, Khakalo A, Hauru L, Korpela A, Orelma H (2018) Conversion of paper to film by ionic liquids: manufacturing process and properties. Cellulose 25:6107–6119

    Article  CAS  Google Scholar 

  • Vergis BR, Krishna RH, Kottam N, Nagabhushana BM, Sharath R, Darukaprasad B (2018) Removal of malachite green from aqueous solution by magnetic CuFe2O4 nano-adsorbent synthesized by one pot solution combustion method. J Nanostruct Chem 8:1–12

    Article  CAS  Google Scholar 

  • Wang X, Ye T, Wang Z, Yang R, Wang R, Ma H, Xiao B, Chu B (2014) Nanofiltration membranes prepared by interfacial polymerization on thin-film nanofibrous composite scaffold. Polymer 55:1358–1366

    Article  CAS  Google Scholar 

  • Wang DC, Yu H, Fan X, Gu J, Ye S, Yao J, Ni Q (2018) High aspect ratio carboxylated cellulose nanofibers crosslinked to robust aerogels for superabsorption-flocculants: paving way from nano-scale to macro-scale. ACS Appl Mater Interfaces 10:20755–20766

    Article  CAS  PubMed  Google Scholar 

  • Weng R, Chen L, Xiao H, Huang F, Lin S, Cao S, Huang L (2017) Preparation and characterization of cellulose nanofiltration membrane through hydrolysis followed by carboxymethylation. Fiber Polym 18:1235–1242

    Article  CAS  Google Scholar 

  • Xia L, Ren J, Wen M, McCutcheon JR (2018) Ceramic-supported thin film composite membrane for organic solvent nanofiltration. J Membr Sci 563:857–863

    Article  CAS  Google Scholar 

  • Xu Q, Chen C, Rosswurm K, Yao T, Janaswamy S (2016) A facile route to prepare cellulose-based films. Carbohydr Polym 149:274–281

    Article  CAS  PubMed  Google Scholar 

  • Xu H, Bronner T, Yamamoto M, Yamane H (2018a) Regeneration of cellulose dissolved in ionic liquid using laser-heated melt-electrospinning. Carbohydr Polym 201:182–188

    Article  CAS  PubMed  Google Scholar 

  • Xu Z, Jiang X, Zhou H, Li J (2018b) Preparation of magnetic hydrophobic polyvinyl alcohol (PVA)-cellulose nanofiber (CNF) aerogels as effective oil absorbents. Cellulose 25:1217–1227

    Article  CAS  Google Scholar 

  • Xu Z, Zhou H, Tan S, Jiang X, Wu W, Shi J, Chen P (2018c) Ultralight super-hydrophobic carbon aerogels based on cellulose nanofibers/poly(vinyl alcohol)/graphene oxide (CNFs/PVA/GO) for highly effective oil-water separation. Beilstein J Nanotechnol 9:508–519

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  • Yang L, Mukhopadhyay A, Jiao YC, Yong Q, Chen L, Xing YJ, Hamel J, Zhu HL (2017a) Ultralight, highly thermally insulating and fire resistant aerogel by encapsulating cellulose nanofibers with two-dimensional MoS2. Nanoscale 9:11452–11462

    Article  CAS  PubMed  Google Scholar 

  • Yang W, Jiao L, Min D, Liu Z, Dai H (2017b) Effects of preparation approaches on optical properties of self-assembled cellulose nanopapers. RSC Adv 7:10463–10468

    Article  CAS  Google Scholar 

  • Yang X, Sun H, Pal A, Bai Y, Shao L (2018) Biomimetic silicification on membrane surface for highly efficient treatments of both oil-in-water emulsion and protein wastewater. ACS Appl Mater Interfaces 10:29982–29991

    Article  CAS  PubMed  Google Scholar 

  • Zhang XF, Feng Y, Huang C, Pan Y, Yao J (2017) Temperature-induced formation of cellulose nanofiber film with remarkably high gas separation performance. Cellulose 24:5649–5656

    Article  CAS  Google Scholar 

  • Zhang XF, Feng Y, Wang Z, Jia M, Yao J (2018a) Fabrication of cellulose nanofibrils/UiO-66-NH2 composite membrane for CO2/N2 separation. J Membr Sci 568:10–16

    Article  CAS  Google Scholar 

  • Zhang XF, Hou T, Chen J, Feng Y, Li B, Gu X, He M, Yao J (2018b) Facilitated transport of CO2 through the transparent and flexible cellulose membrane promoted by fixed-site carrier. ACS Appl Mater Interfaces 10:24930–24936

    Article  CAS  PubMed  Google Scholar 

  • Zhao S, Wang Z (2017) A loose nano-filtration membrane prepared by coating HPAN UF membrane with modified PEI for dye reuse and desalination. J Membr Sci 524:214–224

    Article  CAS  Google Scholar 

  • Zhao Q, Zhu X, Chen B (2018) Stable graphene oxide/poly(ethyleneimine) 3D aerogel with tunable surface charge for high performance selective removal of ionic dyes from water. Chem Eng J 334:1119–1127

    Article  CAS  Google Scholar 

Download references

Acknowledgments

The authors are grateful for financial supports from the Natural Science Key Project of the Jiangsu Higher Education Institutions (15KJA220001), the Natural Science Foundation of Jiangsu Province Youth Fund (BK20180766, BK20170919), and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD). The authors also thank the testing services from Advanced Analysis and Testing Center of Nanjing Forestry University.

Author information

Authors and Affiliations

Authors

Corresponding authors

Correspondence to Ming He or Jianfeng Yao.

Additional information

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Electronic supplementary material

Below is the link to the electronic supplementary material.

Supplementary material 1 (DOCX 2012 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Hou, T., Guo, K., Wang, Z. et al. Glutaraldehyde and polyvinyl alcohol crosslinked cellulose membranes for efficient methyl orange and Congo red removal. Cellulose 26, 5065–5074 (2019). https://doi.org/10.1007/s10570-019-02433-w

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10570-019-02433-w

Keywords

Profiles

  1. Ming He