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A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "2D and Carbon Nanomaterials".

Deadline for manuscript submissions: closed (25 August 2024) | Viewed by 22531

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Special Issue Editors

Dr. Bin Li

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Guest Editor

Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China
Interests: lignocellulose; nanomaterials from biomass; natural polymers; functional materials
Special Issues, Collections and Topics in MDPI journals

Prof. Dr. Chunlin Xu

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Guest Editor

Laboratory of Natural Materials technology, Åbo Akademi University, FI-20500 Turku, Finland
Interests: bio-based materials; nanocellulose; lignin; 3D printing

Prof. Dr. Pedram Fatehi

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Guest Editor

Green Processes Research Centre and Biorefining Research Institute, Lakehead University, Thunder Bay, ON P7B5E1, Canada
Interests: production of advanced cellulose-based materials; modification of lignin and hemicelluloses to produce value-added products; advanced colloid and interface science

Special Issue Information

Dear Colleagues,

Nanomaterials (particularly for cellulose nanomaterials and lignin nanoparticles) derived from biomass have attracted much attention from both academia and industry due to their unique nanostructure and physicochemical properties. Distint from inorganic nanomaterials, nanomaterials from biomass also have good renewability, biocompatibility and biodegrability. Therefore, nanomaterials from biomass have a wide variety of potential applications, such as paper and paperboard for high-quality packaging; rheology modifiers for coatings, paints, foods and drinks; functional fillers for rubber and polymer composites; drug delivery and wound dressing in medicine; moisturizing factors for cosmetics; adsorbents for water treatment; bio-ink for 3D printing; and building blocks for optical, electronic and smart devices. Certainly, the present issues (such as high-cost production, low concentrations of samples, poor re-dispersibility, low durability (particularly in high moisture), and safety evaluation) are still challenging, which should be well addressed.

This Special Issue of Nanomaterials will present comprehensive research outlining the progress in the chemistry, modification, preparation and application of cellulosic nanomaterials and lignin nanoparticles. We invite authors to contribute original research articles and review articles covering the state of the art in the theoretical research and applications of nanomaterials from biomass.

Prof. Dr. Bin Li
Prof. Dr. Chunlin Xu
Prof. Dr. Pedram Fatehi
Guest Editors

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Keywords

biomass
cellulose nanomaterials
nanocellulose
lignin nanoparticles
green chemistry
application

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Published Papers (10 papers)

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Research

Jump to: Review

20 pages, 11854 KiB

Open AccessArticle

Printability Metrics and Engineering Response of HDPE/Si₃N₄ Nanocomposites in MEX Additive Manufacturing

by Vassilis M. Papadakis, Markos Petousis, Nikolaos Michailidis, Maria Spyridaki, Ioannis Valsamos, Apostolos Argyros, Katerina Gkagkanatsiou, Amalia Moutsopoulou and Nectarios Vidakis

Nanomaterials 2024, 14(20), 1680; https://doi.org/10.3390/nano14201680 - 19 Oct 2024

Viewed by 883

Abstract

Herein, silicon nitride (Si₃N₄) was the selected additive to be examined for its reinforcing properties on high-density polyethylene (HDPE) by exploiting techniques of the popular material extrusion (MEX) 3D printing method. Six different HDPE/Si₃N₄ composites with filler percentages ranging between 0.0–10.0 wt. %, having a 2.0 step, were produced initially in compounds, then in filaments, and later in the form of specimens, to be examined by a series of tests. Thermal, rheological, mechanical, structural, and morphological analyses were also performed. For comprehensive mechanical characterization, tensile, flexural, microhardness (M-H), and Charpy impacts were included. Scanning electron microscopy (SME) was used for morphological assessments and microcomputed tomography (μ-CT). Raman spectroscopy was conducted, and the elemental composition was assessed using energy-dispersive spectroscopy (EDS). The HDPE/Si₃N₄ composite with 6.0 wt. % was the one with an enhancing performance higher than the rest of the composites, in the majority of the mechanical metrics (more than 20% in the tensile and flexural experiment), showing a strong potential for Si₃N₄ as a reinforcement additive in 3D printing. This method can be easily industrialized by further exploiting the MEX 3D printing method. Full article

(This article belongs to the Special Issue From Biomass to Nanomaterials)

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14 pages, 3820 KiB

Open AccessEditor’s ChoiceArticle

Regioselectively Carboxylated Cellulose Nanofibril Models from Dissolving Pulp: C6 via TEMPO Oxidation and C2,C3 via Periodate–Chlorite Oxidation

by Mengzhe Guo, James D. Ede, Christie M. Sayes, Jo Anne Shatkin, Nicole Stark and You-Lo Hsieh

Nanomaterials 2024, 14(5), 479; https://doi.org/10.3390/nano14050479 - 6 Mar 2024

Cited by 5 | Viewed by 1646

Abstract

Regioselective C6 and C2,C3 carboxylated cellulose nanofibrils (CNFs) have been robustly generated from dissolving pulp, a readily available source of unmodified cellulose, via stoichiometrically optimized 2,2,6,6-tetramethylpyperidine-1-oxyl (TEMPO)-mediated and sequential sodium periodate-sodium chlorite (PC) oxidation coupled with high-speed blending. Both regioselectively optimized carboxylated CNF series possess the widest ranges of comparable charges (0.72–1.48 mmol/g for T-CNFs vs. 0.72–1.10 mmol/g for PC-CNFs), but similar ranges of thickness (1.3–2.4 nm for T-CNF, 1.8–2.7 nm PC-CNF), widths (4.6–6.6 nm T-CNF, 5.5–5.9 nm PC-CNF), and lengths (254–481 nm T-CNF, 247–442 nm PC-CNF). TEMPO-mediated oxidation is milder and one-pot, thus more time and process efficient, whereas the sequential periodate–chlorite oxidation produces C2,C3 dialdehyde intermediates that are amenable to further chemical functionalization or post-reactions. These two well-characterized regioselectively carboxylated CNF series represent coherent cellulose nanomaterial models from a single woody source and have served as references for their safety study toward the development of a safer-by-design substance evaluation tool. Full article

(This article belongs to the Special Issue From Biomass to Nanomaterials)

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12 pages, 4531 KiB

Open AccessCommunication

Antibacterial Hydrophilic ZnO Microstructure Film with Underwater Oleophobic and Self-Cleaning Antifouling Properties

by Yannan Li, Yu Xue, Jie Wang, Dan Zhang, Yan Zhao and Jun-Jie Liu

Nanomaterials 2024, 14(2), 150; https://doi.org/10.3390/nano14020150 - 10 Jan 2024

Viewed by 1306

Abstract

Super-hydrophilic and oleophobic functional materials can prevent pollution or adsorption by repelling oil, and have good circulation. However, traditional strategies for preparing these functional materials either use expensive fabrication machines or contain possibly toxic organic polymers, which may prohibit the practical application. The research of multifunctional ZnO microstructures or nanoarrays thin films with super-hydrophilic, antifouling, and antibacterial properties has not been reported yet. Moreover, the exploration of underwater oleophobic and self-cleaning antifouling properties in ZnO micro/nanostructures is still in its infancy. Here, we prepared ZnO microstructured films on fluorine-doped tin oxide substrates (F-ZMF) for the development of advanced self-cleaning type super-hydrophilic and oleophobic materials. With the increase of the accelerators, the average size of the F-ZMF microstructures decreased. The F-ZMF shows excellent self-cleaning performance and hydrophilic (water contact angle ≤ 10°) and oleophobic characteristics in the underwater antifouling experiment. Under a dark condition, F-ZMF-4 showed good antibacterial effects against Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli) with inhibition rates of 99.1% and 99.9%, respectively. This study broadens the application scope of ZnO-based material and provides a novel prospect for the development of self-cleaning super-hydrophilic and oleophobic materials. Full article

(This article belongs to the Special Issue From Biomass to Nanomaterials)

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11 pages, 6822 KiB

Open AccessArticle

In-Situ Grown NiMn₂O₄/GO Nanocomposite Material on Nickel Foam Surface by Microwave-Assisted Hydrothermal Method and Used as Supercapacitor Electrode

by Shusen Wang, Xiaomei Du, Sen Liu, Yingqing Fu and Naibao Huang

Nanomaterials 2023, 13(17), 2487; https://doi.org/10.3390/nano13172487 - 4 Sep 2023

Cited by 5 | Viewed by 1590

Abstract

The NiMn₂O₄/graphene oxide (GO) nanocomposite material was in situ grown on the surface of a nickel foam 3D skeleton by combining the solvent method with the microwave-assisted hydrothermal method and annealing; then, its performance was investigated as a superior supercapacitor electrode material. When nickel foam was soaked in GO aqueous or treated in nickel ion and manganese ion solution by the microwave-assisted hydrothermal method and annealing, gauze GO film or flower-spherical NiMn₂O₄ was formed on the nickel foam surface. If the two processes were combined in a different order, the final products on the nickel surface had a remarkably different morphology and phase structure. When GO film was first formed, the final products on the nickel surface were the composite of NiO and Mn₃O₄, while NiMn₂O₄/GO nanocomposite material can be obtained if NiMn₂O₄ was first formed (immersed in 2.5 mg/L GO solution). In a 6M KOH solution, the specific capacitance of the latter reached 700 F/g at 1 A/g which was superior to that of the former (only 35 F/g). However, the latter’s specific capacitance was still inferior to that of in-situ grown NiMn₂O₄ on nickel foam (802 F/g). Though the gauze-formed GO film, almost covering the preformed flower-spherical NiMn₂O₄, can also contribute a certain specific capacitance, it also restricted the electrolyte diffusion and contact with NiMn₂O₄, accounting for the performance decrease of the NiMn₂O₄/GO nanocomposite. A convenient method was raised to fabricate the nanocomposite of carbon and double metal oxides. Full article

(This article belongs to the Special Issue From Biomass to Nanomaterials)

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18 pages, 3735 KiB

Open AccessFeature PaperArticle

Functionalisation of Electrospun Cellulose Acetate Membranes with PEDOT and PPy for Electronic Controlled Drug Release

by Beatriz Lago, Miguel Brito, Cristina M. M. Almeida, Isabel Ferreira and Ana Catarina Baptista

Nanomaterials 2023, 13(9), 1493; https://doi.org/10.3390/nano13091493 - 27 Apr 2023

Cited by 1 | Viewed by 1808

Abstract

Controlled drug release via electrical stimulation from drug-impregnated fibres was studied using electrospun cellulose acetate (CA) membranes and encapsulated ibuprofen (IBU). This research outlines the influence of polypyrrole (PPy) and poly(3,4-ethylenedioxythiophene) (PEDOT)-functionalised CA membranes and their suitability for dermal electronic-controlled drug release. Micro Raman analysis confirmed polymer functionalisation of CA membranes and drug incorporation. Scanning electron microscopy (SEM) images evidenced the presence of PPy and PEDOT coatings. The kinetic of drug release was analysed, and the passive and active release was compared. In the proposed systems, the drug release is controlled by very low electrical potentials. A potential of −0.3 V applied to membranes showed the ibuprofen retention, and a positive potential of +0.3 V, +0.5 V, or +0.8 V, depending on the conductive polymer and membrane configuration, enhanced the drug release. A small adhesive patch was constructed to validate this system for cutaneous application and verified an “ON/OFF” ibuprofen release pattern from membranes. Full article

(This article belongs to the Special Issue From Biomass to Nanomaterials)

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16 pages, 22835 KiB

Open AccessArticle

Valorization of Vegetable Waste from Leek, Lettuce, and Artichoke to Produce Highly Concentrated Lignocellulose Micro- and Nanofibril Suspensions

by Jose Luis Sanchez-Salvador, Mariana P. Marques, Margarida S. C. A. Brito, Carlos Negro, Maria Concepcion Monte, Yaidelin A. Manrique, Ricardo J. Santos and Angeles Blanco

Nanomaterials 2022, 12(24), 4499; https://doi.org/10.3390/nano12244499 - 19 Dec 2022

Cited by 7 | Viewed by 2529

Abstract

Vegetable supply in the world is more than double than vegetable intake, which supposes a significant waste of vegetables, in addition to the agricultural residues produced. As sensitive food products, the reasons for this waste vary from the use of only a part of the vegetable due to its different properties to the product appearance and market image. An alternative high-added-value application for these wastes rich in cellulose could be the reduction in size to produce lignocellulose micro- and nanofibrils (LCMNF). In this sense, a direct treatment of greengrocery waste (leek, lettuce, and artichoke) to produce LCMNFs without the extraction of cellulose has been studied, obtaining highly concentrated suspensions, without using chemicals. After drying the wastes, these suspensions were produced by milling and blending at high shear followed by several passes in the high-pressure homogenizer (up to six passes). The presence of more extractives and shorter fiber lengths allowed the obtention of 5–5.5% leek LCMNF suspensions and 3.5–4% lettuce LCMNF suspensions, whereas for artichoke, only suspensions of under 1% were obtained. The main novelty of the work was the obtention of a high concentration of micro- and nanofiber suspension from the total waste without any pretreatment. These high concentrations are not obtained from other raw materials (wood or annual plants) due to the clogging of the homogenizer, requiring the dilution of the sample up to 1% or the use of chemical pretreatments. Full article

(This article belongs to the Special Issue From Biomass to Nanomaterials)

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13 pages, 2325 KiB

Open AccessEditor’s ChoiceArticle

Amphiphilic Lignin Nanoparticles Made from Lignin-Acrylic Acid-Methyl Methacrylate Copolymers

by Yingchao Wang, Niloofar Alipoormazandarani, Lauren Skye Puumala, Weijue Gao, Shanshan Liu, Fangong Kong, Qiang Wang and Pedram Fatehi

Nanomaterials 2022, 12(15), 2612; https://doi.org/10.3390/nano12152612 - 29 Jul 2022

Cited by 2 | Viewed by 2141

Abstract

In this study, a novel amphiphilic KL-AA-MMA nanoparticle was prepared through the graft copolymerization of kraft lignin (KL) with acrylic acid (AA) and methyl methacrylate (MMA), using potassium persulfate as an initiator in a water/dimethyl sulfoxide solvent medium, which was followed by the nanoprecipitation technique using dimethylformamide as a solvent and deionized water as an antisolvent. The successful graft polymerization was verified by ¹H-nuclear magnetic resonance (NMR), ³¹P-NMR, and Fourier transform infrared (FTIR) analyses; and the grafting yield of the generated KL-AA-MMA copolymer ranged from 68.2% to 96.5%. Transmission electron microscopy (TEM) observation revealed the formation of amorphous KL-AA-MMA nanoparticles. Additionally, KL-AA-MMA9 nanoparticles with the highest yield exhibited the minimum hydrodynamic diameter and polydispersity of 261 nm and 0.153, respectively. Moreover, the amphiphilicity of KL-AA-MMA nanoparticles was significantly improved by the grafting of MMA monomers. Finally, the adsorption performance of KL-AA-MMA nanoparticles at the xylene interface was evaluated by a quartz crystal microbalance with dissipation (QCM-D). The results demonstrated that the most amphiphilic sample, KL-AA-MMA9 nanoparticles, with the smallest hydrodynamic size displayed the highest adsorption on the oil/water interface. This product provides a wide range of applications in oil/water emulsions. Full article

(This article belongs to the Special Issue From Biomass to Nanomaterials)

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16 pages, 27957 KiB

Open AccessArticle

Fabrication and Properties of Tree-Branched Cellulose Nanofibers (CNFs) via Acid Hydrolysis Assisted with Pre-Disintegration Treatment

by Jun Li, Dongyan Liu, Junsheng Li, Fei Yang, Guoxin Sui and Yu Dong

Nanomaterials 2022, 12(12), 2089; https://doi.org/10.3390/nano12122089 - 17 Jun 2022

Cited by 6 | Viewed by 2422

Abstract

In this paper, the novel morphology of cellulose nanofibers (CNFs) with a unique tree-branched structure was discovered by using acid hydrolysis assisted with pre-disintegration treatment from wood pulps. For comparison, the pulps derived from both softwood and hardwood were utilized to extract nanocellulose in order to validate the feasibility of proposed material fabrication technique. The morphology, crystalline structures, chemical structures, and thermal stability of nanocellulose were characterized by means of transmission electron microscopy (TEM), X-ray diffraction (XRD) analysis, Fourier transform infrared spectroscopy (FTIR), as well as thermogravimetric analysis (TGA). Prior to acid hydrolysis, softwood and hardwood pulps underwent the disintegration treatment in the fiber dissociator. It has been found that nanocellulose derived from disintegrated pulps possesses much longer fiber length (approximately 5–6 μm) and more evident tree-branched structures along with lower degree of crystallinity when compared with those untreated counterparts. The maximum mass loss rate of CNFs takes place at the temperature level of approximately 225 °C, and appears to be higher than that of cellulose nanowhiskers (CNWs), which might be attributed to an induced impact of amorphous content. On the other hand, disintegration treatment is quite beneficial to the enhancement of tensile strength of nanocellulose films. This study elaborates a new route of material fabrication toward the development of well-tailored tree-branched CNFs in order to broaden the potential widespread applications of nanocellulose with diverse morphological structures. Full article

(This article belongs to the Special Issue From Biomass to Nanomaterials)

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Review

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34 pages, 4141 KiB

Open AccessEditor’s ChoiceReview

Development of Processes and Catalysts for Biomass to Hydrocarbons at Moderate Conditions: A Comprehensive Review

by Reem Shomal and Ying Zheng

Nanomaterials 2023, 13(21), 2845; https://doi.org/10.3390/nano13212845 - 27 Oct 2023

Cited by 1 | Viewed by 2463

Abstract

This comprehensive review explores recent catalyst advancements for the hydrodeoxygenation (HDO) of aromatic oxygenates derived from lignin, with a specific focus on the selective production of valuable aromatics under moderate reaction conditions. It addresses critical challenges in bio-crude oil upgrading, encompassing issues related to catalyst deactivation from coking, methods to mitigate deactivation, and techniques for catalyst regeneration. The study investigates various oxygenates found in bio-crude oil, such as phenol, guaiacol, anisole, and catechol, elucidating their conversion pathways during HDO. The review emphasizes the paramount importance of selectively generating arenes by directly cleaving C–O bonds while avoiding unwanted ring hydrogenation pathways. A comparative analysis of different bio-crude oil upgrading processes underscores the need to enhance biofuel quality for practical applications. Additionally, the review focuses on catalyst design for HDO. It compares six major catalyst categories, including metal sulfides, transition metals, metal phosphides, nitrides, carbides, and oxides, to provide insights for efficient bio-crude oil upgrading toward sustainable and eco-friendly energy alternatives. Full article

(This article belongs to the Special Issue From Biomass to Nanomaterials)

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22 pages, 4632 KiB

Open AccessReview

Tailoring Functionality of Nanocellulose: Current Status and Critical Challenges

by Yidong Zhang, Wangfang Deng, Meiyan Wu, Mehdi Rahmaninia, Chunlin Xu and Bin Li

Nanomaterials 2023, 13(9), 1489; https://doi.org/10.3390/nano13091489 - 27 Apr 2023

Cited by 15 | Viewed by 3783

Abstract

Nanocellulose (NC) isolated from natural cellulose resources, which mainly includes cellulose nanofibril (CNF) and cellulose nanocrystal (CNC), has garnered increased attention in recent decades due to its outstanding physical and chemical properties. Various chemical modifications have been developed with the aim of surface-modifying NC for highly sophisticated applications. This review comprehensively summarizes the chemical modifications applied to NC so far in order to introduce new functionalities to the material, such as silanization, esterification, oxidation, etherification, grafting, coating, and others. The new functionalities obtained through such surface-modification methods include hydrophobicity, conductivity, antibacterial properties, and absorbability. In addition, the incorporation of NC in some functional materials, such as films, wearable sensors, cellulose nanospheres, aerogel, hydrogels, and nanocomposites, is discussed in relation to the tailoring of the functionality of NC. It should be pointed out that some issues need to be addressed during the preparation of NC and NC-based materials, such as the low reactivity of these raw materials, the difficulties involved in their scale-up, and their high energy and water consumption. Over the past decades, some methods have been developed, such as the use of pretreatment methods, the adaptation of low-cost starting raw materials, and the use of environmentally friendly chemicals, which support the practical application of NC and NC-based materials. Overall, it is believed that as a green, sustainable, and renewable nanomaterial, NC is will be suitable for large-scale applications in the future. Full article

(This article belongs to the Special Issue From Biomass to Nanomaterials)

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