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Polymers
Special Issues
Cellulose-Based Polymeric Materials
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Cellulose-Based Polymeric Materials

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Biobased and Biodegradable Polymers".

Deadline for manuscript submissions: 25 March 2025 | Viewed by 8835

Special Issue Editors

Dr. Maria Graça Rasteiro

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Guest Editor
Chemical Process Engineering and Forest Products Research Centre (CIEPQPF), Department of Chemical Engineering, University of Coimbra, Rua Sílvio Lima, 3030-790 Coimbra, Portugal
Interests: particle technology, including particle characterization; multiphase processes, including modelling and experimental; rheology of suspensions; tomographic techniques for multiphase flow visualization; aggregation/flocculation of particles; valorization of ligno-cellulosic materials—development of natural polyelectrolytes and lignin-based surfactants; remediation of soils; microplastics identification and removal
Special Issues, Collections and Topics in MDPI journals
Dr. Luis Alves

E-Mail Website
Guest Editor
CIEPQPF—Chemical Process Engineering and Forest Products Research Centre, Department of Chemical Engineering, University of Coimbra, Rua Sílvio Lima, 3030-790 Coimbra, Portugal
Interests: cellulose chemistry; cellulose dissolution and regeneration; nanocellulose production and characterization; cellulose and nanocellulose-based organic–inorganic hybrid materials; bio-based polyelectrolytes from lignocellulosic materials; lignin-based materials; rheology; surfactants; polymer–surfactant association; microscopy
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Biopolymer-based materials are, in general, environmentally friendly materials, which can be obtained from renewable sources. Following a circular economy principle, cellulose can be obtained from biomass residues from forests or crop production. Cellulose, being the most abundant biopolymer on the planet, is an obvious choice to produce materials with favourable properties for a wide range of applications, such as biomedical applications, environmental applications, food packaging and electronic devices, thus being a logical substitute to petroleum-based polymers, especially plastics. Cellulose is also a remarkable starting material for chemical modification, due to the large available hydroxyl groups in its structure. Thus, the preparation of water-soluble cellulose derivatives is suitable as rheology modifiers, flocculants, etc., depending on the derivatization introduced. The derivatization can be carried out via different methods, leading to partially or fully dissolved cellulose. Other important classes of cellulosic materials are nanocelluloses (cellulose nanocrystals (CNC), cellulose nanofibrils (CNF) and bacterial cellulose (BC)). This class of biobased nanomaterials possesses outstanding properties and finds application in multiple areas.

In this Special Issue, the objective is to bring together recent advances in the field of cellulose-based materials, including the use of different cellulosic materials, wastes valorisation, preparation procedures, and application in different fields, including industrial application.

Dr. Maria Graça Rasteiro
Dr. Luis Alves
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • sustainability
  • bio-based materials
  • wastes valorisation
  • nanocelluloses
  • cellulose matrixes
  • bioflocculants
  • cellulose derivatives
  • cellulose dissolution
  • biomass fractionation

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Published Papers (7 papers)

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Research

17 pages, 1412 KiB  
Article
Adsorption and Bulk Assembly of Quaternized Hydroxyethylcellulose–Anionic Surfactant Complexes on Negatively Charged Substrates
by Maud Nivard, Francisco Ortega, Ramón G. Rubio and Eduardo Guzmán
Polymers 2025, 17(2), 207; https://doi.org/10.3390/polym17020207 - 15 Jan 2025
Viewed by 543
Abstract
This study examines the adsorption and bulk assembly behaviour of quaternized hydroxyethylcellulose ethoxylate (QHECE)–sodium dodecyl sulphate (SDS) complexes on negatively charged substrates. Due to its quaternized structure, QHECE, which is used in several industries, including cosmetics, exhibits enhanced electrostatic interactions. The phase behaviour [...] Read more.
This study examines the adsorption and bulk assembly behaviour of quaternized hydroxyethylcellulose ethoxylate (QHECE)–sodium dodecyl sulphate (SDS) complexes on negatively charged substrates. Due to its quaternized structure, QHECE, which is used in several industries, including cosmetics, exhibits enhanced electrostatic interactions. The phase behaviour and adsorption mechanisms of QHECE–SDS complexes are investigated using model substrates that mimic the wettability and surface charge of damaged hair fibres. Two preparation methodologies, high-concentration mixing and gradient-free mixing, were employed to examine their impact on the complex equilibrium, phase behaviour, and adsorption properties of the complexes. The measurements of turbidity, electrophoretic mobility, and conductivity demonstrate the existence of nonequilibrium dynamics during the mixing process, which exert a significant influence on the structural and functional characteristics of the complexes. The quartz crystal microbalance with dissipation monitoring (QCM-D) was employed to investigate the adsorption of the complexes onto the substrates. The results demonstrated the critical role of intermediate SDS concentrations in enhancing deposition. The findings emphasise the importance of formulation and preparation protocols in designing stable, high-performance cosmetic products. This research advances our understanding of polyelectrolyte–surfactant interactions and provides insights into optimising QHECE-based formulations. Full article
(This article belongs to the Special Issue Cellulose-Based Polymeric Materials)
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14 pages, 6447 KiB  
Article
Acid-Hydrolysis-Assisted Cellulose Nanocrystal Isolation from Acacia mearnsii de Wild. Wood Kraft Pulp
by Daniel Tavares de Farias, Jalel Labidi, Cristiane Pedrazzi, Darci Alberto Gatto, Pedro Henrique Gonzalez de Cademartori, Carline Andréa Welter, Gabriela Teixeira da Silva and Tielle Moraes de Almeida
Polymers 2024, 16(23), 3371; https://doi.org/10.3390/polym16233371 - 29 Nov 2024
Viewed by 692
Abstract
Cellulose nanocrystals (CNC) receive great attention for their physical and optical properties, high surface area, high tensile strength, rigidity (Young’s modulus up to 140 GPa), and ease of surface modification. However, controlling the properties of CNC is still challenging, given the wide variety [...] Read more.
Cellulose nanocrystals (CNC) receive great attention for their physical and optical properties, high surface area, high tensile strength, rigidity (Young’s modulus up to 140 GPa), and ease of surface modification. However, controlling the properties of CNC is still challenging, given the wide variety of pulp sources and the complexity of finding suitable processing conditions. In the present study, acid hydrolysis efficiently isolated CNC from wood Acacia mearnsii brown kraft pulp (AMKP). Initially, the AMKP was delignified by the treatment with acidified sodium chlorite. The Acacia mearnsii kraft pulp obtained was then subjected to acid hydrolysis with sulfuric acid at concentrations of 50 to 58% 45 °C for 60 min. The hydrolysate was sonicated in an ultrasonic processor for 30 min. The chemical composition was determined by Fourier transform infrared spectroscopy (FTIR), crystallinity by X-ray diffraction (XRD), zeta potential by Zetasizer ZS equipment, thermal stability by thermogravimetric analysis (TGA), and morphology by transmission electron microscopy (TEM) to verify the effect of acid concentration on the yield and properties of CNC. The optimization of the isolation process demonstrated that the maximum yield of 41.95% can be obtained when AMWP was hydrolyzed with sulfuric acid at a concentration of 54%. It was possible to isolate CNC with a crystallinity index between 71.66% and 81.76%, with the onset of thermal degradation at 240 °C; zeta potential of −47.87 to 57.23 mV; and rod-like morphology, with lengths and widths between 181.70 nm and 260.24 nm and 10.36 nm and 11.06 nm, respectively. Sulfuric acid concentration significantly affected the yield of acid hydrolysis, allowing the isolation of CNC with variable dimensions, high thermal stability, high crystallinity index, and great colloidal stability in aqueous medium. Full article
(This article belongs to the Special Issue Cellulose-Based Polymeric Materials)
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20 pages, 4639 KiB  
Article
Customising Sustainable Bio-Based Polyelectrolytes: Introduction of Charged and Hydrophobic Groups in Cellulose
by Solange Magalhães, María José Aliaño-González, Pedro F. Cruz, Rose Rosenberg, Dirk Haffke, Magnus Norgren, Luís Alves, Bruno Medronho and Maria da Graça Rasteiro
Polymers 2024, 16(22), 3105; https://doi.org/10.3390/polym16223105 - 5 Nov 2024
Cited by 1 | Viewed by 1085
Abstract
Cellulose has been widely explored as a sustainable alternative to synthetic polymers in industrial applications, thanks to its advantageous properties. The introduction of chemical modifications on cellulose structure, focusing on cationic and hydrophobic modifications, can enhance its functionality and expand the range of [...] Read more.
Cellulose has been widely explored as a sustainable alternative to synthetic polymers in industrial applications, thanks to its advantageous properties. The introduction of chemical modifications on cellulose structure, focusing on cationic and hydrophobic modifications, can enhance its functionality and expand the range of applications. In the present work, cationization was carried out through a two-step process involving sodium periodate oxidation followed by a reaction with the Girard T reagent, yielding a degree of substitution for cationic groups (DScationic) between 0.3 and 1.8. Hydrophobic modification was achieved via esterification with fatty acids derived from commercial plant oils, using an enzyme-assisted, environmentally friendly method. Lipase-catalysed hydrolysis, optimised at 0.25% enzyme concentration and with a 1 h reaction time, produced an 84% yield of fatty acids, confirmed by FTIR and NMR analyses. The degree of substitution for hydrophobic groups (DShydrophobic) ranged from 0.09 to 0.66. The molecular weight (MW) of the modified cellulose derivatives varied from 1.8 to 141 kDa. This dual modification strategy enables the creation of cellulose-based polymers with controlled electrostatic and hydrophobic characteristics, customisable for specific industrial applications. Our approach presents a sustainable and flexible solution for developing cellulose derivatives tailored to diverse industrial needs. Full article
(This article belongs to the Special Issue Cellulose-Based Polymeric Materials)
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21 pages, 3775 KiB  
Article
On the Valorization of Olive Oil Pomace: A Sustainable Approach for Methylene Blue Removal from Aqueous Media
by El Mokhtar Saoudi Hassani, Hugo Duarte, João Brás, Abdeslam Taleb, Mustapha Taleb, Zakia Rais, Alireza Eivazi, Magnus Norgren, Anabela Romano and Bruno Medronho
Polymers 2024, 16(21), 3055; https://doi.org/10.3390/polym16213055 - 30 Oct 2024
Cited by 1 | Viewed by 781
Abstract
Currently, industrial water pollution represents a significant global challenge, with the potential to adversely impact human health and the integrity of ecosystems. The continuous increase in global consumption has resulted in an exponential rise in the use of dyes, which have become one [...] Read more.
Currently, industrial water pollution represents a significant global challenge, with the potential to adversely impact human health and the integrity of ecosystems. The continuous increase in global consumption has resulted in an exponential rise in the use of dyes, which have become one of the major water pollutants, causing significant environmental impacts. In order to address these concerns, a number of wastewater treatment methods have been developed, with a particular focus on physicochemical approaches, such as adsorption. The objective of this study is to investigate the potential of a bio-based material derived from olive oil pomace (OOP) as an environmentally friendly bio-adsorbent for the removal of methylene blue (MB), a cationic dye commonly found in textile effluents. The biobased material was initially characterized by determining the point of zero charge (pHpzc) and using scanning electron microscopy (SEM), X-ray diffraction (XRD), and Fourier transform infrared spectroscopy (FTIR). Subsequently, a comprehensive analysis was conducted, evaluating the impact of specific physicochemical parameters on MB adsorption, which included a thorough examination of the kinetic and thermodynamic aspects. The adsorption process was characterized using Langmuir, Freundlich, Brunauer-Emmett-Teller (BET), and Dubinin Radushkevich (D-R) isotherms. The results suggest that the equilibrium of adsorption is achieved within ca. 200 min, following pseudo-second-order kinetics. The optimal conditions, including adsorbent mass, temperature, bulk pH, and dye concentration, yielded a maximum adsorption capacity of ca. 93% (i.e., 428 mg g−1) for a pomace concentration of 450 mg L−1. The results suggest a monolayer adsorption process with preferential electrostatic interactions between the dye and the pomace adsorbent. This is supported by the application of Langmuir, BET, Freundlich, and D-R isotherm models. The thermodynamic analysis indicates that the adsorption process is spontaneous and exothermic. This work presents a sustainable solution for mitigating MB contamination in wastewater streams while simultaneously valorizing OOP, an agricultural by-product that presents risks to human health and the environment. In conclusion, this approach offers an innovative ecological alternative to synthetic adsorbents. Full article
(This article belongs to the Special Issue Cellulose-Based Polymeric Materials)
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13 pages, 9094 KiB  
Article
Preparation and Application of Responsive Nanocellulose Composites
by Yanhui Zhou, Lu Zhang and Yuan Li
Polymers 2024, 16(11), 1446; https://doi.org/10.3390/polym16111446 - 21 May 2024
Viewed by 837
Abstract
Cellulose nanofibrils/poly(N-Isopropylacrylamide) semi-interpenetrating networks (MMCNF-PNAs) were synthesized using an in situ fabrication (semi-IPN). The polymerization of N-isopropylacrylamide (NIPAM) (free radical) was conducted in the presence of magnetic modified cellulose nanofibrils (MMCNFs). The adsorption behaviors and surface morphology of the synthesized adsorbents were investigated [...] Read more.
Cellulose nanofibrils/poly(N-Isopropylacrylamide) semi-interpenetrating networks (MMCNF-PNAs) were synthesized using an in situ fabrication (semi-IPN). The polymerization of N-isopropylacrylamide (NIPAM) (free radical) was conducted in the presence of magnetic modified cellulose nanofibrils (MMCNFs). The adsorption behaviors and surface morphology of the synthesized adsorbents were investigated systematically. The adsorption behaviors of the as-prepared MMCNF-PNA towards methylene blue (MB, as the model contaminant) dye was studied, and the optimal adsorption conditions were also studied. The adsorption processes could be well fitted using pseudo-second-order and Elovich kinetic models. Meanwhile, Langmuir and Freundlich isotherm models were used to fit the adsorption which occurred at 25, 37 and 65 °C. The corresponding results showed that the Freundlich isotherm model fitted the adsorption process better, indicating that the dye’s adsorption happened via heterogeneous adsorptive energies on the prepared MMCNF-PNAs. Their desorption and reusability were also studied to verify magnetic responsivity. To sum up, MMCNF-PNAs are promising magnetic and thermal stimuli-responsive adsorbents, showing a controlled adsorption/desorption process. Full article
(This article belongs to the Special Issue Cellulose-Based Polymeric Materials)
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11 pages, 2503 KiB  
Article
A High-Proton Conductivity All-Biomass Proton Exchange Membrane Enabled by Adenine and Thymine Modified Cellulose Nanofibers
by Chong Xie, Runde Yang, Xing Wan, Haorong Li, Liangyao Ge, Xiaofeng Li and Guanglei Zhao
Polymers 2024, 16(8), 1060; https://doi.org/10.3390/polym16081060 - 11 Apr 2024
Cited by 1 | Viewed by 1261
Abstract
Nanocellulose fiber materials were considered promising biomaterials due to their excellent biodegradability, biocompatibility, high hydrophilicity, and cost-effectiveness. However, their low proton conductivity significantly limited their application as proton exchange membranes. The methods previously reported to increase their proton conductivity often introduced non-biodegradable groups [...] Read more.
Nanocellulose fiber materials were considered promising biomaterials due to their excellent biodegradability, biocompatibility, high hydrophilicity, and cost-effectiveness. However, their low proton conductivity significantly limited their application as proton exchange membranes. The methods previously reported to increase their proton conductivity often introduced non-biodegradable groups and compounds, which resulted in the loss of the basic advantages of this natural polymer in terms of biodegradability. In this work, a green and sustainable strategy was developed to prepare cellulose-based proton exchange membranes that could simultaneously meet sustainability and high-performance criteria. Adenine and thymine were introduced onto the surface of tempo-oxidized nanocellulose fibers (TOCNF) to provide many transition sites for proton conduction. Once modified, the proton conductivity of the TOCNF membrane increased by 31.2 times compared to the original membrane, with a specific surface area that had risen from 6.1 m²/g to 86.5 m²/g. The wet strength also increased. This study paved a new path for the preparation of environmentally friendly membrane materials that could replace the commonly used non-degradable ones, highlighting the potential of nanocellulose fiber membrane materials in sustainable applications such as fuel cells, supercapacitors, and solid-state batteries. Full article
(This article belongs to the Special Issue Cellulose-Based Polymeric Materials)
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13 pages, 3060 KiB  
Article
Kinetics of Periodate-Mediated Oxidation of Cellulose
by Nazmun Sultana, Ulrica Edlund, Chandan Guria and Gunnar Westman
Polymers 2024, 16(3), 381; https://doi.org/10.3390/polym16030381 - 30 Jan 2024
Cited by 5 | Viewed by 2764
Abstract
The oxidation of cellulose to dialdehyde cellulose (DAC) is a process that has received increased interest during recent years. Herein, kinetic modeling of the reaction with sodium periodate as an oxidizing agent was performed to quantify rate-limiting steps and overall kinetics of the [...] Read more.
The oxidation of cellulose to dialdehyde cellulose (DAC) is a process that has received increased interest during recent years. Herein, kinetic modeling of the reaction with sodium periodate as an oxidizing agent was performed to quantify rate-limiting steps and overall kinetics of the cellulose oxidation reaction. Considering a pseudo-first-order reaction, a general rate expression was derived to elucidate the impact of pH, periodate concentration, and temperature on the oxidation of cellulose and concurrent formation of cellulose degradation products. Experimental concentration profiles were utilized to determine the rate constants for the formation of DAC (k1), degradation constant of cellulose (k2), and degradation of DAC (k3), confirming that the oxidation follows a pseudo-first-order reaction. Notably, the increase in temperature has a more pronounced effect on k1 compared to the influence of IO4− concentration. In contrast, k2 and k3 display minimal changes in response to IO4− concentration but increase significantly with increasing temperature. The kinetic model developed may help with understanding the rate-limiting steps and overall kinetics of the cellulose oxidation reaction, providing valuable information for optimizing the process toward a faster reaction with higher yield of the target product. Full article
(This article belongs to the Special Issue Cellulose-Based Polymeric Materials)
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