Research Article | | Peer-Reviewed

Biocomposite Films Based on Carrageenan and Graphite: Elaboration and Characterization

Received: 26 September 2025     Accepted: 6 December 2025     Published: 10 July 2026
Views:       Downloads:
Abstract

This work focuses on the development and characterization of novel biodegradable composite materials combining carrageenan matrices with graphite reinforcement. Graphite, a material of significant contemporary interest due to its exceptional electrical conductivity, thermal stability, and mechanical strength, was exfoliated using an optimized mechanical ultrasound method in aqueous medium to produce few-layer graphene sheets with minimal defects. The exfoliation parameters, including sonication time (2hour), amplitude (80%), and temperature control (maintained below 40°C), were carefully calibrated to ensure reproducible results. Carrageenans, sustainable biopolymers, were extracted from two red seaweed species: Kappaphycus alvarezii (Cottonii) and Eucheuma denticulatum (Spinosum), collected from coastal regions of Madagascar. The extraction protocol involved sequential steps of washing, alkaline treatment, filtration, precipitation with isopropanol, and final drying, yielding high-purity κ- and ι-carrageenan types respectively. Composite films were fabricated using solution mixing and casting-evaporation techniques, involving dissolution of carrageenan in distilled water at 80°C and homogeneous dispersion of exfoliated graphite via probe sonication. The mixtures were then cast onto glass plates and dried under controlled conditions (25°C, 50% RH) for 48h, producing uniform films with thicknesses ranging from 80mm to 120mm. The resulting bio(nano)composite films were systematically characterized using Thermogravimetric Analysis (TGA), X-ray Diffraction (XRD), and Fourier Transform Infrared Spectroscopy (FT-IR). TGA revealed a significant increase in degradation temperature from 242°C for pure Carr-Co to 278°C for composites with 2% filler, representing a 36°C improvement in thermal stability. XRD analysis showed characteristic graphite peaks at 2θ = 26.53° with d-spacing values of approximately 0.34nm, confirming the preservation of crystalline structure after processing. FT-IR spectra confirmed successful integration of graphite within the carrageenan matrix through observed band shifts and reduced hydroxyl stretching intensities. These promising results highlight the potential of graphite-reinforced carrageenan composites for advanced applications including sustainable packaging materials with enhanced barrier properties, biomedical scaffolds for tissue engineering with improved structural integrity, and biodegradable electronics with tunable conductivity. Future work will focus on comprehensive mechanical property evaluation using dynamic mechanical analysis, detailed biodegradability studies in simulated environmental conditions, systematic investigation of water vapor permeability, and preliminary scale-up feasibility assessment for industrial production. Additionally, the antimicrobial properties and cytotoxicity profiles of these composites will be explored to broaden their applicability in medical and food packaging sectors.

Published in Composite Materials (Volume 10, Issue 2)
DOI 10.11648/j.cm.20261002.11
Page(s) 17-24
Creative Commons

This is an Open Access article, distributed under the terms of the Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution and reproduction in any medium or format, provided the original work is properly cited.

Copyright

Copyright © The Author(s), 2026. Published by Science Publishing Group

Keywords

Red Seaweed, Carrageenan, Graphite, Graphene, Casting-evaporation, Bio(nano)composites

References
[1] Wang, Guoxiu & Yang. (2008) Facile synthesis and characterization of graphene nanosheets. The Journal of Physical Chemistry C, vol. 112, no. 12, pp. 1946-1955, 2008.
[2] M. El Achaby. (2012). Graphene-Thermoplastic Polymer Nanocomposites: Fabrication and Study of Structural, Thermal, Rheological, and Mechanical Properties. PhD thesis, Mohammed V-Agdal University, Faculty of Sciences, Rabat.
[3] R. KAKEK. (2022). Utilization of Natural Composite Materials. PhD thesis, Kasdi Merbah University, Ouargla.
[4] Scherba, Craig & Montreuil. (2018). Geology and economics of the giant Molo graphite deposit, southern Madagascar.
[5] D. Chung. (1987). Exfoliation of graphite. Journal of materials science, vol. 22, pp. 4190-4198.
[6] R. Croft. (1960). Lamellar compounds of graphite. Quarterly Reviews, Chemical Society, vol. 14, no. 1, pp. 1-45.
[7] K. S. Novoselov, Geim. (2004). Electric field effect in atomically thin carbon films. Science, vol. 306, no. 5696, pp. 666-669.
[8] A. K. Geim & K. S. Novoselov. (2007). The rise of graphene. Nature materials, vol. 6, no. 3, pp. 183-191.
[9] Q. Wang, Qianqian & Ji. (2020). Structure and properties of polylactic acid biocomposite films reinforced with cellulose nanofibrils. Molecules, vol. 25, no. 14, p. 3306.
[10] A. A. Balandin, S. Ghosh, W. Bao, I. Calizo, D. Teweldebrhan, F. Miao, & C. N. Lau. (2008). Superior thermal conductivity of single-layer graphene. Nanoletters, vol. 8, no. 3, pp. 902-907.
[11] G. Todinanahary, Behivoke. (2016). Inventory and Feasibility Study of Sites Suitable for Algal Cultivation, Sea Cucumber Farming, and the Management of Octopus and Crab Harvesting in the Atsimo Andrefana Region. MHSA¯PRU (Contrat n 166/C/PIC2/2016) Report, Toliara, Madagascar.
[12] W. H. Organization. (2022). Report of the expert meeting on food safety for seaweed: current status and future perspectives. Rome, 28-29 October 2021.
[13] M. Rinaudo. (2002). Alginates and carrageenans. Actualit Chimique, no. 11/12, pp. 35-38.
[14] M. Khotimchenko, V. Tiasto, A. Kalitnik, M. Begun, R. Khotimchenko, E. Leonteva, I. Bryukhovetskiy, & Y. Khotimchenko. (2020). Antitumor potential of carrageenans from marine red algae. Carbohydrate Polymers, vol. 246, p. 116568.
[15] Souza, Bartolomeu WS & Cerqueira, Miguel A and Bourbon, Ana I and Pinheiro, Ana C and Martins, Joana T and Teixeira, José A and Coimbra, Manuel A and Vicente, António A. (2012). Chemical characterization and antioxidant activity of sulfated polysaccharide from the red seaweed Gracilaria birdiae. Food Hydrocolloids, vol. 27, no. 2, pp. 287-292.
[16] Utilization of Marine Polysaccharides: Development of Nanocomposites and Synthesis of Doped Graphene. PhD thesis, Normandie Universit.
[17] S. Toumi, Yahoum. (2022). Synthesis and physicochemical evaluation of octenylsuccinated kappa-carrageenan: Conventional versus microwave heating. Carbohydrate Polymers, vol. 286, p. 119310.
[18] Modification of the Physicochemical Properties of Carrageenans through Purification and Characterization of Carrageenan Sulfatases. PhD thesis, Universit Pierre et Marie Curie-UPMC.
[19] M. Abdorreza, Robal. (2012). Physicochemical, thermal, and rheological properties of acid-hydrolyzed sago (metroxylon sagu) starch. LWT-Food Science and Technology, vol. 46, no. 1, pp. 135-141.
[20] J. T. Martins, Bourbon. (2013). Biocomposite films based on $kappa$-carrageenan/locust bean gum blends and clays: physical and antimicrobial properties. Food and Bioprocess Technology, vol. 6, pp. 2081-2092.
[21] H. Jdidi, Fourati. (2021). Exploring the optical and dielectric properties of bifunctional and trifunctional epoxy polymers. Polymer, vol. 228, p. 123882.
[22] X. Lu, Detrez. (2021). Identification of elastic properties of interphase and interface in graphene-polymer nanocomposites by atomistic simulations. Composites Science and Technology, vol. 213, p. 108943.
[23] Development of Nanocomposites Based on Renewable-Source Polymers¯Optimization of Barrier and Transport Properties. Theses.fr, PhD thesis, Reims.
[24] A. Ibrahim, Klopocinska. (2021). Graphene-based nanocomposites: Synthesis, mechanical properties, and characterizations. Polymers, vol. 13, no. 17, p. 2869.
[25] A. Popova. (2017). Crystallographic analysis of graphite by x-ray diffraction. Coke and Chemistry, vol. 60, pp. 361-365.
[26] N. A. A. Ghani, Othaman. (2019) Impact of purification on iota carrageenan as solid polymer electrolyte. Arabian journal of chemistry, vol. 12, no. 3, pp. 370-376.
[27] A. Michel, M. Mestdagh, & M. Axelos. (1997). Physicochemical properties of carrageenan gels in presence of various cations. International Journal of Biological Macromolecules, vol. 21, no. 1-2, pp. 195-200.
[28] M. D. Torres, Chenlo. (2018). Structural features and water sorption isotherms of carrageenans: A prediction model for hybrid carrageenans. Carbohydrate Polymers, vol. 180, pp. 72-80.
[29] C. Bellion. (1979). Utilisation d'enzymes pour la caractérisation des carraghénanes kappa et iota.
[30] L. Pereira, Critchley. (2009). A comparative analysis of phycocolloids produced by underutilized versus industrially utilized carrageenophytes (gigartinales, rhodophyta). Journal of Applied Phycology, vol. 21, pp. 599-605.
[31] R. Chitra, Sathya. (2019). Synthesis and characterization of iota-carrageenan solid biopolymer electrolytes for electrochemical applications. Ionics, vol. 25, no. 5, pp. 2147-2157.
Cite This Article
  • APA Style

    Miller, R. M., Ernest, M. O. L. J., Tsarambita, O. B., Maka, O. D., Joyeux, H. T., et al. (2026). Biocomposite Films Based on Carrageenan and Graphite: Elaboration and Characterization. Composite Materials, 10(2), 17-24. https://doi.org/10.11648/j.cm.20261002.11

    Copy | Download

    ACS Style

    Miller, R. M.; Ernest, M. O. L. J.; Tsarambita, O. B.; Maka, O. D.; Joyeux, H. T., et al. Biocomposite Films Based on Carrageenan and Graphite: Elaboration and Characterization. Compos. Mater. 2026, 10(2), 17-24. doi: 10.11648/j.cm.20261002.11

    Copy | Download

    AMA Style

    Miller RM, Ernest MOLJ, Tsarambita OB, Maka OD, Joyeux HT, et al. Biocomposite Films Based on Carrageenan and Graphite: Elaboration and Characterization. Compos Mater. 2026;10(2):17-24. doi: 10.11648/j.cm.20261002.11

    Copy | Download

  • @article{10.11648/j.cm.20261002.11,
      author = {Rabearison Mizea Miller and Mamiarisitraka Oligina Lalatina Jean Ernest and Oudinot Bricharles Tsarambita and Olivier Dimbiniaina Maka and Heriniaina Theophyle Joyeux and Maherizo Tiandrainy Gedice and Heriarivelo Risite},
      title = {Biocomposite Films Based on Carrageenan and Graphite: Elaboration and Characterization},
      journal = {Composite Materials},
      volume = {10},
      number = {2},
      pages = {17-24},
      doi = {10.11648/j.cm.20261002.11},
      url = {https://doi.org/10.11648/j.cm.20261002.11},
      eprint = {https://article.sciencepublishinggroup.com/pdf/10.11648.j.cm.20261002.11},
      abstract = {This work focuses on the development and characterization of novel biodegradable composite materials combining carrageenan matrices with graphite reinforcement. Graphite, a material of significant contemporary interest due to its exceptional electrical conductivity, thermal stability, and mechanical strength, was exfoliated using an optimized mechanical ultrasound method in aqueous medium to produce few-layer graphene sheets with minimal defects. The exfoliation parameters, including sonication time (2hour), amplitude (80%), and temperature control (maintained below 40°C), were carefully calibrated to ensure reproducible results. Carrageenans, sustainable biopolymers, were extracted from two red seaweed species: Kappaphycus alvarezii (Cottonii) and Eucheuma denticulatum (Spinosum), collected from coastal regions of Madagascar. The extraction protocol involved sequential steps of washing, alkaline treatment, filtration, precipitation with isopropanol, and final drying, yielding high-purity κ- and ι-carrageenan types respectively. Composite films were fabricated using solution mixing and casting-evaporation techniques, involving dissolution of carrageenan in distilled water at 80°C and homogeneous dispersion of exfoliated graphite via probe sonication. The mixtures were then cast onto glass plates and dried under controlled conditions (25°C, 50% RH) for 48h, producing uniform films with thicknesses ranging from 80mm to 120mm. The resulting bio(nano)composite films were systematically characterized using Thermogravimetric Analysis (TGA), X-ray Diffraction (XRD), and Fourier Transform Infrared Spectroscopy (FT-IR). TGA revealed a significant increase in degradation temperature from 242°C for pure Carr-Co to 278°C for composites with 2% filler, representing a 36°C improvement in thermal stability. XRD analysis showed characteristic graphite peaks at 2θ = 26.53° with d-spacing values of approximately 0.34nm, confirming the preservation of crystalline structure after processing. FT-IR spectra confirmed successful integration of graphite within the carrageenan matrix through observed band shifts and reduced hydroxyl stretching intensities.	These promising results highlight the potential of graphite-reinforced carrageenan composites for advanced applications including sustainable packaging materials with enhanced barrier properties, biomedical scaffolds for tissue engineering with improved structural integrity, and biodegradable electronics with tunable conductivity. Future work will focus on comprehensive mechanical property evaluation using dynamic mechanical analysis, detailed biodegradability studies in simulated environmental conditions, systematic investigation of water vapor permeability, and preliminary scale-up feasibility assessment for industrial production. Additionally, the antimicrobial properties and cytotoxicity profiles of these composites will be explored to broaden their applicability in medical and food packaging sectors.},
     year = {2026}
    }
    

    Copy | Download

  • TY  - JOUR
    T1  - Biocomposite Films Based on Carrageenan and Graphite: Elaboration and Characterization
    AU  - Rabearison Mizea Miller
    AU  - Mamiarisitraka Oligina Lalatina Jean Ernest
    AU  - Oudinot Bricharles Tsarambita
    AU  - Olivier Dimbiniaina Maka
    AU  - Heriniaina Theophyle Joyeux
    AU  - Maherizo Tiandrainy Gedice
    AU  - Heriarivelo Risite
    Y1  - 2026/07/10
    PY  - 2026
    N1  - https://doi.org/10.11648/j.cm.20261002.11
    DO  - 10.11648/j.cm.20261002.11
    T2  - Composite Materials
    JF  - Composite Materials
    JO  - Composite Materials
    SP  - 17
    EP  - 24
    PB  - Science Publishing Group
    SN  - 2994-7103
    UR  - https://doi.org/10.11648/j.cm.20261002.11
    AB  - This work focuses on the development and characterization of novel biodegradable composite materials combining carrageenan matrices with graphite reinforcement. Graphite, a material of significant contemporary interest due to its exceptional electrical conductivity, thermal stability, and mechanical strength, was exfoliated using an optimized mechanical ultrasound method in aqueous medium to produce few-layer graphene sheets with minimal defects. The exfoliation parameters, including sonication time (2hour), amplitude (80%), and temperature control (maintained below 40°C), were carefully calibrated to ensure reproducible results. Carrageenans, sustainable biopolymers, were extracted from two red seaweed species: Kappaphycus alvarezii (Cottonii) and Eucheuma denticulatum (Spinosum), collected from coastal regions of Madagascar. The extraction protocol involved sequential steps of washing, alkaline treatment, filtration, precipitation with isopropanol, and final drying, yielding high-purity κ- and ι-carrageenan types respectively. Composite films were fabricated using solution mixing and casting-evaporation techniques, involving dissolution of carrageenan in distilled water at 80°C and homogeneous dispersion of exfoliated graphite via probe sonication. The mixtures were then cast onto glass plates and dried under controlled conditions (25°C, 50% RH) for 48h, producing uniform films with thicknesses ranging from 80mm to 120mm. The resulting bio(nano)composite films were systematically characterized using Thermogravimetric Analysis (TGA), X-ray Diffraction (XRD), and Fourier Transform Infrared Spectroscopy (FT-IR). TGA revealed a significant increase in degradation temperature from 242°C for pure Carr-Co to 278°C for composites with 2% filler, representing a 36°C improvement in thermal stability. XRD analysis showed characteristic graphite peaks at 2θ = 26.53° with d-spacing values of approximately 0.34nm, confirming the preservation of crystalline structure after processing. FT-IR spectra confirmed successful integration of graphite within the carrageenan matrix through observed band shifts and reduced hydroxyl stretching intensities.	These promising results highlight the potential of graphite-reinforced carrageenan composites for advanced applications including sustainable packaging materials with enhanced barrier properties, biomedical scaffolds for tissue engineering with improved structural integrity, and biodegradable electronics with tunable conductivity. Future work will focus on comprehensive mechanical property evaluation using dynamic mechanical analysis, detailed biodegradability studies in simulated environmental conditions, systematic investigation of water vapor permeability, and preliminary scale-up feasibility assessment for industrial production. Additionally, the antimicrobial properties and cytotoxicity profiles of these composites will be explored to broaden their applicability in medical and food packaging sectors.
    VL  - 10
    IS  - 2
    ER  - 

    Copy | Download

Author Information
  • Sections