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A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Synthesis, Interfaces and Nanostructures".

Deadline for manuscript submissions: closed (31 December 2021) | Viewed by 39477

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Prof. Dr. Takuya Kitaoka

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Department of Agro-Environmental Sciences, Graduate School of Bioresource and Bioenvironmental Sciences, Kyushu University, Fukuoka 819-0395, Japan
Interests: cellulose; chitin; chitosan; polysaccharides; nanofibers; hybrid nanomaterials; interfacial catalysis; organocatalysis; green chemistry; biomaterials; biointerfaces; cell engineering; biomedical applications

Special Issue Information

Dear Colleagues,

Natural polysaccharides, such as cellulose, chitin, and starch, possess hierarchical nanoarchitectures, e.g., crystalline, nanofibrous, needle-like, helical, folded, and chain-aligned structures, in which macromolecular components assemble in a regular and organized manner during biosynthesis and physicochemical processing. Nanocellulose is one of the most promising nanomaterials in practical applications due to its high aspect ratio, high elastic modulus, high transparency, and low thermal expansion coefficient. Chitin nanofibers are also expected to be used to produce advanced nanomaterials for cosmetics and biomedical applications. Research and development of natural polysaccharides can be classified into two categories: (1) greener alternatives to existing products, from ecological and sustainability viewpoints; and (2) emerging functional nanomaterials, from scientific encounters with the unknown.

Both approaches are important to advancing the further utilization of natural polysaccharides; however, in this Special Issue, I would like to focus on the second topic, which includes the unexpected new functions arising from the inherent nanoarchitectures of natural nano-organized polysaccharides, all of which will provide new insights into and concepts for polysaccharide-driven nanomaterial chemistry and engineering.

We welcome original research papers, communications, and short reviews. Potential topics include, but are not limited to:

crystalline-structure-triggered novel functions of nano-organized polysaccharides;
nanomorphology-triggered novel functions of nano-organized polysaccharides;
nanointerface-triggered novel functions of nano-organized polysaccharides; and
nanocomposite-triggered novel functions of nano-organized polysaccharides.

In any case, nano-organized polysaccharides themselves are expected to play critical roles in the emerging functions of nanomaterials. I look forward to your contribution.

Prof. Dr. Takuya Kitaoka
Guest Editor

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Keywords

nanocellulose
cellulose nanofibers
chitin and chitosan nanofibers
polysaccharide nanostructures
functional nanomaterials
functional biointerfaces
methodologies for the design and preparation of nano-organized polysaccharides
challenges in exploring new functions of nano-organized polysaccharides

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Published Papers (12 papers)

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Editorial

Jump to: Research, Review

3 pages, 171 KiB

Open AccessEditorial

Emerging Functions of Nano-Organized Polysaccharides

by Takuya Kitaoka

Nanomaterials 2022, 12(8), 1277; https://doi.org/10.3390/nano12081277 - 8 Apr 2022

Viewed by 1444

Abstract

Natural polysaccharides, such as cellulose and chitin, possess unique hierarchical nanoarchitectures, e [...] Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

Research

Jump to: Editorial, Review

12 pages, 1736 KiB

Open AccessArticle

Facile Preparation of Mechanically Robust and Functional Silica/Cellulose Nanofiber Gels Reinforced with Soluble Polysaccharides

by Marco Beaumont, Elisabeth Jahn, Andreas Mautner, Stefan Veigel, Stefan Böhmdorfer, Antje Potthast, Wolfgang Gindl-Altmutter and Thomas Rosenau

Nanomaterials 2022, 12(6), 895; https://doi.org/10.3390/nano12060895 - 8 Mar 2022

Cited by 3 | Viewed by 2760

Abstract

Nanoporous silica gels feature extremely large specific surface areas and high porosities and are ideal candidates for adsorption-related processes, although they are commonly rather fragile. To overcome this obstacle, we developed a novel, completely solvent-free process to prepare mechanically robust CNF-reinforced silica nanocomposites via the incorporation of methylcellulose and starch. Significantly, the addition of starch was very promising and substantially increased the compressive strength while preserving the specific surface area of the gels. Moreover, different silanes were added to the sol/gel process to introduce in situ functionality to the CNF/silica hydrogels. Thereby, CNF/silica hydrogels bearing carboxyl groups and thiol groups were produced and tested as adsorber materials for heavy metals and dyes. The developed solvent-free sol/gel process yielded shapable 3D CNF/silica hydrogels with high mechanical strength; moreover, the introduction of chemical functionalities further widens the application scope of such materials. Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

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12 pages, 2139 KiB

Open AccessEditor’s ChoiceArticle

Combination of Polysaccharide Nanofibers Derived from Cellulose and Chitin Promotes the Adhesion, Migration and Proliferation of Mouse Fibroblast Cells

by Tomoka Noda, Mayumi Hatakeyama and Takuya Kitaoka

Nanomaterials 2022, 12(3), 402; https://doi.org/10.3390/nano12030402 - 26 Jan 2022

Cited by 14 | Viewed by 3597

Abstract

Extracellular matrix (ECM) as a structural and biochemical scaffold to surrounding cells plays significant roles in cell adhesion, migration, proliferation and differentiation. Herein, we show the novel combination of TEMPO-oxidized cellulose nanofiber (TOCNF) and surface-N-deacetylated chitin nanofiber (SDCtNF), respectively, having carboxylate and amine groups on each crystalline surface, for mouse fibroblast cell culture. The TOCNF/SDCtNF composite scaffolds demonstrated characteristic cellular behavior, strongly depending on the molar ratios of carboxylates and amines of polysaccharide NFs. Pure TOCNF substrate exhibited good cell attachment, although intact carboxylate-free CNF made no contribution to cell adhesion. By contrast, pure SDCtNF induced crucial cell aggregation to form spheroids; nevertheless, the combination of TOCNF and SDCtNF enhanced cell attachment and subsequent proliferation. Molecular blend of carboxymethylcellulose and acid-soluble chitosan made nearly no contribution to cell culture behavior. The wound healing assay revealed that the polysaccharide combination markedly promoted skin repair for wound healing. Both of TOCNF and SDCtNF possessed rigid nanofiber nanoarchitectures with native crystalline forms and regularly-repeated functional groups, of which such structural characteristics would provide a potential for developing cell culture scaffolds having ECM functions, possibly promoting good cellular adhesion, migration and growth in the designated cellular microenvironments. Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

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12 pages, 3314 KiB

Open AccessFeature PaperArticle

Polydopamine Doping and Pyrolysis of Cellulose Nanofiber Paper for Fabrication of Three-Dimensional Nanocarbon with Improved Yield and Capacitive Performances

by Luting Zhu, Kojiro Uetani, Masaya Nogi and Hirotaka Koga

Nanomaterials 2021, 11(12), 3249; https://doi.org/10.3390/nano11123249 - 30 Nov 2021

Cited by 9 | Viewed by 3930

Abstract

Biomass-derived three-dimensional (3D) porous nanocarbons have attracted much attention due to their high surface area, permeability, electrical conductivity, and renewability, which are beneficial for various electronic applications, including energy storage. Cellulose, the most abundant and renewable carbohydrate polymer on earth, is a promising precursor to fabricate 3D porous nanocarbons by pyrolysis. However, the pyrolysis of cellulosic materials inevitably causes drastic carbon loss and volume shrinkage. Thus, polydopamine doping prior to the pyrolysis of cellulose nanofiber paper is proposed to fabricate the 3D porous nanocarbons with improved yield and volume retention. Our results show that a small amount of polydopamine (4.3 wt%) improves carbon yield and volume retention after pyrolysis at 700 °C from 16.8 to 26.4% and 15.0 to 19.6%, respectively. The pyrolyzed polydopamine-doped cellulose nanofiber paper has a larger specific surface area and electrical conductivity than cellulose nanofiber paper that without polydopamine. Owing to these features, it also affords a good specific capacitance up to 200 F g⁻¹ as a supercapacitor electrode, which is higher than the recently reported cellulose-derived nanocarbons. This method provides a pathway for the effective fabrication of high-performance cellulose-derived 3D porous nanocarbons. Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

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11 pages, 3703 KiB

Open AccessArticle

Nanocellulose Xerogel as Template for Transparent, Thick, Flame-Retardant Polymer Nanocomposites

by Wataru Sakuma, Shuji Fujisawa, Lars A. Berglund and Tsuguyuki Saito

Nanomaterials 2021, 11(11), 3032; https://doi.org/10.3390/nano11113032 - 12 Nov 2021

Cited by 12 | Viewed by 4015

Abstract

Cellulose nanofibers (CNFs) have excellent properties, such as high strength, high specific surface areas (SSA), and low coefficients of thermal expansion (CTE), making them a promising candidate for bio-based reinforcing fillers of polymers. A challenge in the field of CNF-reinforced composite research is to produce strong and transparent CNF/polymer composites that are sufficiently thick for use as load-bearing structural materials. In this study, we successfully prepared millimeter-thick, transparent CNF/polymer composites using CNF xerogels, with high porosity (~70%) and high SSA (~350 m² g⁻¹), as a template for monomer impregnation. A methacrylate was used as the monomer and was cured by UV irradiation after impregnation into the CNF xerogels. The CNF xerogels effectively reinforced the methacrylate polymer matrix, resulting in an improvement in the flexural modulus (up to 546%) and a reduction in the CTE value (up to 78%) while maintaining the optical transparency of the matrix polymer. Interestingly, the composites exhibited flame retardancy at high CNF loading. These unique features highlight the applicability of CNF xerogels as a reinforcing template for producing multifunctional and load-bearing polymer composites. Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

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12 pages, 4905 KiB

Open AccessArticle

Highly Stable Pickering Emulsions with Xylan Hydrate Nanocrystals

by Shanyong Wang and Zhouyang Xiang

Nanomaterials 2021, 11(10), 2558; https://doi.org/10.3390/nano11102558 - 29 Sep 2021

Cited by 20 | Viewed by 2770

Abstract

Xylan is a highly abundant plant-based biopolymer. Original xylans in plants are in an amorphous state, but deacetylated and low-branched xylan can form a crystalline structure with water molecules. The utilizations of xylan have been limited to bulk applications either with inconsistency and uncertainty or with extensive chemical derivatization due to the insufficient studies on its crystallization. The applications of xylan could be greatly broadened in advanced green materials if xylan crystals are effectively utilized. In this paper, we show a completely green production of nano-sized xylan crystals and propose their application in forming Pickering emulsions. The branches of xylan were regulated during the separation step to controllably induce the formation of xylan hydrate crystals. Xylan hydrate nanocrystals (XNCs) with a uniform size were successfully produced solely by a mild ultrasonic treatment. XNCs can be adsorbed onto oil–water interfaces at a high density to form highly stable Pickering emulsions. The emulsifying properties of XNCs were comparable to some synthetic emulsifiers and better than some other common biopolymer nanocrystals, demonstrating that XNCs have great potential in industrial emulsification. Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

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11 pages, 1333 KiB

Open AccessArticle

Doxorubicin Embedded into Nanofibrillated Bacterial Cellulose (NFBC) Produces a Promising Therapeutic Outcome for Peritoneally Metastatic Gastric Cancer in Mice Models via Intraperitoneal Direct Injection

by Hidenori Ando, Takashi Mochizuki, Amr S. Abu Lila, Shunsuke Akagi, Kenji Tajima, Kenji Fujita, Taro Shimizu, Yu Ishima, Tokuo Matsushima, Takatomo Kusano and Tatsuhiro Ishida

Nanomaterials 2021, 11(7), 1697; https://doi.org/10.3390/nano11071697 - 28 Jun 2021

Cited by 8 | Viewed by 2805

Abstract

Natural materials such as bacterial cellulose are gaining interest for their use as drug-delivery vehicles. Herein, the utility of nanofibrillated bacterial cellulose (NFBC), which is produced by culturing a cellulose-producing bacterium (Gluconacetobacter intermedius NEDO-01) in a medium supplemented with carboxymethylcellulose (CMC) that is referred to as CM-NFBC, is described. Recently, we demonstrated that intraperitoneal administration of paclitaxel (PTX)-containing CM-NFBC efficiently suppressed tumor growth in a peritoneally disseminated cancer xenograft model. In this study, to confirm the applicability of NFBC in cancer therapy, a chemotherapeutic agent, doxorubicin (DXR), embedded into CM-NFBC, was examined for its efficiency to treat a peritoneally disseminated gastric cancer via intraperitoneal administration. DXR was efficiently embedded into CM-NFBC (DXR/CM-NFBC). In an in vitro release experiment, 79.5% of DXR was released linearly into the peritoneal wash fluid over a period of 24 h. In the peritoneally disseminated gastric cancer xenograft model, intraperitoneal administration of DXR/CM-NFBC induced superior tumor growth inhibition (TGI = 85.5%) by day 35 post-tumor inoculation, compared to free DXR (TGI = 62.4%). In addition, compared with free DXR, the severe side effects that cause body weight loss were lessened via treatment with DXR/CM-NFBC. These results support the feasibility of CM-NFBC as a drug-delivery vehicle for various anticancer agents. This approach may lead to improved therapeutic outcomes for the treatment of intraperitoneally disseminated cancers. Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

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12 pages, 2225 KiB

Open AccessArticle

Molecular and Crystal Structure of a Chitosan−Zinc Chloride Complex

by Toshifumi Yui, Takuya Uto and Kozo Ogawa

Nanomaterials 2021, 11(6), 1407; https://doi.org/10.3390/nano11061407 - 26 May 2021

Cited by 5 | Viewed by 2833

Abstract

We determined the molecular and packing structure of a chitosan–ZnCl₂ complex by X-ray diffraction and linked-atom least-squares. Eight D-glucosamine residues—composed of four chitosan chains with two-fold helical symmetry, and four ZnCl₂ molecules—were packed in a rectangular unit cell with dimensions a = 1.1677 nm, b = 1.7991 nm, and c = 1.0307 nm (where c is the fiber axis). We performed exhaustive structure searches by examining all of the possible chain packing modes. We also comprehensively searched the positions and spatial orientations of the ZnCl₂ molecules. Chitosan chains of antiparallel polarity formed zigzag-shaped chain sheets, where N2···O6, N2···N2, and O6···O6 intermolecular hydrogen bonds connected the neighboring chains. We further refined the packing positions of the ZnCl₂ molecules by theoretical calculations of the crystal models, which suggested a possible coordination scheme of Zn(II) with an O6 atom. Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

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12 pages, 3065 KiB

Open AccessEditor’s ChoiceArticle

Enzymatic Preparation and Characterization of Spherical Microparticles Composed of Artificial Lignin and TEMPO-Oxidized Cellulose Nanofiber

by Naoya Fukuda, Mayumi Hatakeyama and Takuya Kitaoka

Nanomaterials 2021, 11(4), 917; https://doi.org/10.3390/nano11040917 - 3 Apr 2021

Cited by 8 | Viewed by 3781

Abstract

A one-pot and one-step enzymatic synthesis of submicron-order spherical microparticles composed of dehydrogenative polymers (DHPs) of coniferyl alcohol as a typical lignin precursor and TEMPO-oxidized cellulose nanofibers (TOCNFs) was investigated. Horseradish peroxidase enzymatically catalyzed the radical coupling of coniferyl alcohol in an aqueous suspension of TOCNFs, resulting in the formation of spherical microparticles with a diameter and sphericity index of approximately 0.8 μm and 0.95, respectively. The ζ-potential of TOCNF-functionalized DHP microspheres was about −40 mV, indicating that the colloidal systems had good stability. Nanofibrous components were clearly observed on the microparticle surface by scanning electron microscopy, while some TOCNFs were confirmed to be inside the microparticles by confocal laser scanning microscopy with Calcofluor white staining. As both cellulose and lignin are natural polymers known to biodegrade, even in the sea, these woody TOCNF−DHP microparticle nanocomposites were expected to be promising alternatives to fossil resource-derived microbeads in cosmetic applications. Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

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9 pages, 2244 KiB

Open AccessCommunication

Enhancement of Luminance in Powder Electroluminescent Devices by Substrates of Smooth and Transparent Cellulose Nanofiber Films

by Shota Tsuneyasu, Rikuya Watanabe, Naoki Takeda, Kojiro Uetani, Shogo Izakura, Keitaro Kasuya, Kosuke Takahashi and Toshifumi Satoh

Nanomaterials 2021, 11(3), 697; https://doi.org/10.3390/nano11030697 - 10 Mar 2021

Cited by 10 | Viewed by 3135

Abstract

Powder electroluminescent (EL) devices with an electric field type excitation are surface light sources that are expected to have a wide range of practical applications, owing to their high environmental resistance; however, their low luminance has hindered their use. A clarification of the relationship between the properties of the film substrates and the electroluminescence is important to drastically improve light extraction efficiency. In this study, powder EL devices with different substrates of various levels of surface roughness and different optical transmittances were fabricated to quantitatively evaluate the relationships between the substrate properties and the device characteristics. A decrease in the surface roughness of the substrate caused a clear increase in both the current density and the luminance. The luminance was found to have a direct relationship with the optical transmittance of the substrates. The powder EL device, which was based on a cellulose nanofiber film and was the smoothest and most transparent substrate investigated, showed the highest luminance (641 cd/cm²) when 300 V was applied at 1 kHz. Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

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11 pages, 2793 KiB

Open AccessCommunication

Thermal Conductivity Analysis of Chitin and Deacetylated-Chitin Nanofiber Films under Dry Conditions

by Jiahao Wang, Keitaro Kasuya, Hirotaka Koga, Masaya Nogi and Kojiro Uetani

Nanomaterials 2021, 11(3), 658; https://doi.org/10.3390/nano11030658 - 8 Mar 2021

Cited by 15 | Viewed by 2617

Abstract

Chitin, a natural polysaccharide polymer, forms highly crystalline nanofibers and is expected to have sophisticated engineering applications. In particular, for development of next-generation heat-transfer and heat-insulating materials, analysis of the thermal conductivity is important, but the thermal conductivity properties of chitin nanofiber materials have not been reported. The thermal conductivity properties of chitin nanofiber materials are difficult to elucidate without excluding the effect of adsorbed water and analyzing the influence of surface amino groups. In this study, we aimed to accurately evaluate the thermal conductivity properties of chitin nanofiber films by changing the content of surface amino groups and measuring the thermal diffusivity under dry conditions. Chitin and deacetylated-chitin nanofiber films with surface deacetylation of 5.8% and 25.1% showed in-plane thermal conductivity of 0.82 and 0.73 W/mK, respectively. Taking into account that the films had similar crystalline structures and almost the same moisture contents, the difference in the thermal conductivity was concluded to only depend on the amino group content on the fiber surfaces. Our methodology for measuring the thermal diffusivity under conditioned humidity will pave the way for more accurate analysis of the thermal conductivity performance of hydrophilic materials. Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

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Review

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29 pages, 5817 KiB

Open AccessReview

Construction of Functional Materials in Various Material Forms from Cellulosic Cholesteric Liquid Crystals

by Kazuma Miyagi and Yoshikuni Teramoto

Nanomaterials 2021, 11(11), 2969; https://doi.org/10.3390/nano11112969 - 5 Nov 2021

Cited by 18 | Viewed by 4002

Abstract

Wide use of bio-based polymers could play a key role in facilitating a more sustainable society because such polymers are renewable and ecofriendly. Cellulose is a representative bio-based polymer and has been used in various materials. To further expand the application of cellulose, it is crucial to develop functional materials utilizing cellulosic physicochemical properties that are acknowledged but insufficiently applied. Cellulose derivatives and cellulose nanocrystals exhibit a cholesteric liquid crystal (ChLC) property based on rigidity and chirality, and this property is promising for constructing next-generation functional materials. The form of such materials is an important factor because material form is closely related with function. To date, researchers have reported cellulosic ChLC materials with a wide range of material forms—such as films, gels, mesoporous materials, and emulsions—for diverse functions. We first briefly review the fundamental aspects of cellulosic ChLCs. Then we comprehensively review research on cellulosic ChLC functional materials in terms of their material forms. Thus, this review provides insights into the creation of novel cellulosic ChLC functional materials based on material form designed toward the expanded application of cellulosics. Full article

(This article belongs to the Special Issue Emerging Functions of Nano-Organized Polysaccharides)

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