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The effect of electric charge density of polyacrylamide (PAM) on properties of PAM/cellulose nanofibril composite films

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Abstract

Poly(acrylamides) (PAMs) with various anionic and cationic charge densities from −1.64 to +0.98 meq/g but similar molecular weights were synthesized through radical polymerization. One of the aqueous PAM solutions and an aqueous dispersion of 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofibril (TOCN) were mixed at various PAM/TOCN weight ratios, and self-standing PAM/TOCN composite films were prepared by casting and drying. Because nonionic and cationic PAM molecules may have had some attractive interactions with anionic TOCN elements, the visual appearances and particle sizes of the mixtures varied depending on the charge densities of PAMs. In particular, PAM molecules with electric charge densities with +0.54 and +0.98 meq/g formed polyelectrolyte complexes with anionic TOCN elements, resulting in formation of large agglomerates in the aqueous mixtures. The PAM/TOCN composite films at weight ratios of 10/90 and 25/75 had higher Young’s moduli and tensile strengths than those of 100 % TOCN film, when PAMs with charge densities from −1.64 to +0.54 were used. The PAM/TOCN composite films at the weight ratio of 10/90 had elongations at break similar to that of 100 % TOCN film, resulting in higher work of fracture values or ductile properties, whereas the PAM/TOCN composite films at the weight ratio of 25/75 were rather brittle.

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References

  • Bernabé P, Peniche C, Argüelles-Monal W (2005) Swelling behavior of chitosan/pectin polyelectrolyte complex membranes. Effect of thermal cross-linking. Polym Bull 55:367–375

    Article  Google Scholar 

  • Chen J, Heitmann JA, Hubbe MA (2003) Dependency of polyelectrolyte complex stoichiometry on the order of addition. 1. Effect of salt concentration during streaming current titrations with strong polyacid and polybase. Colloids Surf A 223:215–230

    Article  CAS  Google Scholar 

  • Dong XM, Revol JF, Gray DG (1998) Effect of microcrystallite preparation conditions on the formation of colloid crystals of cellulose. Cellulose 5:19–32

    Article  CAS  Google Scholar 

  • Endo R, Saito T, Isogai A (2013) TEMPO-oxidized cellulose nanofibril/poly(vinyl alcohol) composite drawn fibers. Polymer 54:935–941

    Article  CAS  Google Scholar 

  • Fujisawa S, Ikeuchi T, Takeuchi M, Saito T, Isogai A (2012) Superior reinforcement effect of TEMPO-oxidized cellulose nanofibrils in polystyrene matrix: optical, thermal, and mechanical studies. Biomacromolecules 13:2188–2194

    Article  CAS  Google Scholar 

  • Fujisawa S, Saito T, Kimura S, Iwata T, Isogai A (2013) Surface engineering of ultrafine cellulose nanofibrils toward polymer nanocomposite materials. Biomacromolecules 14:1541–1546

    Article  CAS  Google Scholar 

  • Habibi Y, Lucia LA, Rojas OJ (2010) Cellulose nanocrystals: chemistry, self-assembly, and applications. Chem Rev 110:3479–3600

    Article  CAS  Google Scholar 

  • Henriksson M, Berglund LA, Isaksson P, Lindström T, Nishino T (2008) Cellulose nanopaper structures of high toughness. Biomacromolecules 9:1579–1585

    Article  CAS  Google Scholar 

  • Hirota M, Furihata K, Saito T, Kawada T, Isogai A (2010) Glucose/glucuronic acid alternating co-polysaccharides prepared from TEMPO-oxidized native celluloses by surface peeling. Angew Chem Int Ed 49:7670–7672

    Article  CAS  Google Scholar 

  • Horward KA, Dash PR, Read ML, Ward K, Tomkins LM, Nazarova O, Ulbrich K, Seymour LW (2000) Influence of hydrophilicity of cationic polymers on the biophysical properties of polyelectrolyte complexes formed by self-assembly with DNA. BBA-Gen Subj 1475:245–255

    Article  Google Scholar 

  • Isogai A (2013) Wood nanocelluloses: fundamentals and applications as new bio-based nanomaterials. J Wood Sci 59:449–459

    Article  CAS  Google Scholar 

  • Isogai A, Saito T, Fukuzumi H (2011) TEMPO-oxidized cellulose nanofibers. Nanoscale 3:71–85

    Article  CAS  Google Scholar 

  • Johnson RK, Zink-Sharp A, Renneckar SH, Glasser WG (2009) A new bio-based nanocompoiste: fibrillated TEMPO-oxidized celluloses in hydroxypropylcellulose matrix. Cellulose 16:227–238

    Article  CAS  Google Scholar 

  • Klemm D, Kramer F, Moritz S, Lindström T, Ankerfors M, Gray D, Dorris A (2011) Nanocelluloses: a new family of nature-based materials. Angew Chem Int Ed 50:5438–5466

    Article  CAS  Google Scholar 

  • Kurihara T, Isogai A (2014) Properties of poly(acrylamide)/TEMPO-oxidized cellulose nanofibril composite films. Cellulose 21:291–299

    Article  CAS  Google Scholar 

  • Li Z, Renneckar S, Barone JR (2010) Nanocomposites prepared by in situ enzymatic polymerization of phenol with TEMPO-oxidized nanocellulose. Cellulose 17:57–68

    Article  Google Scholar 

  • Liu A, Walther A, Ikkala O, Belova L, Berglund LA (2011) Clay nanopaper with tough cellulose nanofiber matrix for fire retardancy and gas barrier functions. Biomacromolecules 12:633–641

    Article  CAS  Google Scholar 

  • Michaels AS (1965) Polyelectrolyte complexes. Ind Eng Chem 57:32–40

    Article  CAS  Google Scholar 

  • Okita Y, Saito T, Isogai A (2010) Entire surface oxidation of various cellulose microfibrils by TEMPO-mediated oxidation. Biomacromolecules 11:1696–1700

    Article  CAS  Google Scholar 

  • Saito T, Nishiyama Y, Putaux JL, Vignon M, Isogai A (2006) Homogeneous suspensions of individualized microfibrils from TEMPO-catalyzed oxidation of native cellulose. Biomacromolecules 7:1687–1691

    Article  CAS  Google Scholar 

  • Saito T, Kimura S, Nishiyama Y, Isogai A (2007) Cellulose nanofibers prepared by TEMPO-mediated oxidation of native cellulose. Biomacromolecules 8:2485–2491

    Article  CAS  Google Scholar 

  • Sehaqui H, Liu A, Zhou Q, Berglund LA (2010) Fast preparation procedure for large, flat cellulose and cellulose/inorganic nanopaper structures. Biomacromolecules 11:2195–2198

    Article  CAS  Google Scholar 

  • Shinoda R, Saito T, Okita Y, Isogai A (2012) Relationship between length and degree of polymerization of TEMPO-oxidized cellulose nanofibrils. Biomacromolecules 13:842–849

    Article  CAS  Google Scholar 

  • Siró I, Plackett D (2010) Microfibrillated cellulose and new nanocompoiste materials: a review. Cellulose 17:459–494

    Article  Google Scholar 

  • Takahashi M, Iyoda K, Miyauchi T, Ohkido S, Tahashi M, Wakita K, Kajitani N, Kurachi M, Hotta K (2009) Preparation and characterization of Eu:Ti codoped LiNbO3 films prepared by the sol–gel method. J Appl Phys 106:044102

    Article  Google Scholar 

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Acknowledgments

This research was supported by Core Research for Evolutional Science and Technology (CREST) of Japan Science and Technology Agency (JST).

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Correspondence to Akira Isogai.

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Kurihara, T., Isogai, A. The effect of electric charge density of polyacrylamide (PAM) on properties of PAM/cellulose nanofibril composite films. Cellulose 22, 499–506 (2015). https://doi.org/10.1007/s10570-014-0478-x

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  • DOI: https://doi.org/10.1007/s10570-014-0478-x

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