Preparation of tannic acid-reinforced cellulose nanofiber composites for all-water-based high-performance wood adhesives.

Traditional adhesives easily release toxic gases during the preparation process or apply to wood composite products, which have adverse effects on the human body and the environment. Herein, an all-water-based high-performance wood adhesive is prepared using TEMPO-oxidized cellulose nanofiber (TOCNF), acrylamide (AM), and tannic acid (TA) through free radical polymerization. Different characteristics of the prepared composites, including morphology, injectability, and adhesion properties, have been investigated. Results showed that the TA/TOCNF/PAM composite has excellent injectability. The addition of TA can enhance the lap shear strength of the TA/TOCNF/PAM composites and with the increment of TA content, the lap shear strength gradually decreases. The formation of effective hydrogen bonds and Van der Waals interaction among the rich functional groups in the composite, lead to strong lap shear strength on different substrates. The composite with 5.0 g of AM, 5.0 g of the TOCNF suspension and 0.1 g TA possesses a high lap shear strength of 10.5 MPa on wood and 1.5 MPa on aluminium. Based on strong adhesion properties and excellent injectability, the TA/TOCNF/PAM composites have great potential in the furniture construction and building industries.

A review of cellulose-based catechol-containing functional materials for advanced applications.

With the increment in global energy consumption and severe environmental pollution, it is urgently needed to explore green and sustainable materials. Inspired by nature, catechol groups in mussel adhesion proteins have been successively understood and utilized as novel biomimetic materials. In parallel, cellulose presents a wide class of functional materials rating from macro-scale to nano-scale components. The cross-over among both research fields alters the introduction of impressive materials with potential engineering properties, where catechol-containing materials supply a general stage for the functionalization of cellulose or cellulose derivatives. In this review, the role of catechol groups in the modification of cellulose and cellulose derivatives is discussed. A broad variety of advanced applications of cellulose-based catechol-containing materials, including adhesives, hydrogels, aerogels, membranes, textiles, pulp and papermaking, composites, are presented. Furthermore, some critical remaining challenges and opportunities are studied to mount the way toward the rational purpose and applications of cellulose-based catechol-containing materials.

Biocompatible, Injectable, and Self-Healing Poly(N-vinylpyrrolidone)/Carboxymethyl Cellulose Hydrogel for Drug Release.

Hydrogels have drawn intensive attention as fascinating materials for biomedicine. However, fabricating hydrogels with injectable and self-healing properties remains a challenge. Herein, we reported a biocompatible poly(N-vinylpyrrolidone)/carboxymethyl cellulose (PVP/CMC) hydrogel with excellent injectable and self-healing properties. The PVP/CMC hydrogel exhibits good biocompatible, injectable, and self-healing properties. The sol-gel transition of PVP/CMC hydrogels demonstrates an outstanding self-healing behavior, and the bisected hydrogels can self-heal within 30 s. The hydrogels have a good swelling ratio, and the swelling ratio increases with increasing amount of CMC in PVP and reaches a maximum of 2850% at a 1.0:1.5 PVP and CMC ratio. In addition, the hydrogel possesses excellent drug release capacity, and its drug release rate reaches 70%. Moreover, the release of 4-aminosalicylic acid (4-ASA) in the hydrogel can be controlled by adjusting the proportion of the hydrogel. The PVP/CMC hydrogel with excellent biocompatible, injectable, and self-healing properties has great potential for applications in drug release.

Development of Biocompatible Mussel-Inspired Cellulose-Based Underwater Adhesives.

Conventional adhesives have poor underwater adhesion and harm to human health and the environment during their use, which largely limits their practical applications. Herein, we synthesized cellulose-based adhesives with underwater adhesion and biocompatibility by grafting N-(3,4-dihydroxyphenethyl)methacrylamide into the cellulose chain via atom transfer radical polymerization (ATRP). FTIR, 1H NMR, and XPS analyses ensured the successful preparation of the cellulose-based adhesive polymers. The different properties of the prepared adhesives, including swelling ratio, adhesion strength, and biocompatibility are examined. Results found that the lap shear strength is enhanced by increasing the catechol content. When catechol content is 27.2 mol %, cellulose-based adhesive with the addition of Fe3+ possesses a strong lap shear strength of 2.13 MPa in a dry environment, 0.10 MPa underwater, and 0.16 MPa under seawater for iron substrate, respectively. In addition, the cell culture test demonstrated that the prepared adhesives have outstanding biocompatibility. The cellulose-based adhesives with underwater adhesion and biocompatibility have potential applications in biomedicine, electronic engineering, and construction fields.

Recent advances in TEMPO-oxidized cellulose nanofibers: Oxidation mechanism, characterization, properties and applications.

Cellulose is the richest renewable polymer source on the earth. TEMPO-mediated oxidized cellulose nanofibers are deduced from enormously available wood biomass and functionalized with carboxyl groups. The preparation procedure of TOCNFs is more environmentally friendly compared to other cellulose, for example, MFC and CNCs. Due to the presence of functional carboxyl groups, TOCNF-based materials have been studied widely in different fields, including biomedicine, wastewater treatment, bioelectronics and others. In this review, the TEMPO oxidation mechanism, the properties and applications of TOCNFs are elaborated. Most importantly, the recent advanced applications and the beneficial role of TOCNFs in the various abovementioned fields are discussed. Furthermore, the performances and research progress on the fabrication of TOCNFs are summarized. It is expected that this timely review will help further research on the invention of novel material from TOCNFs and its applications in different advanced fields, including biomedicine, bioelectronics, wastewater treatment, and the energy sector.

Preparation of lignin-based hydrogels, their properties and applications.

Polymers obtained from biomass are a concerning alternative to petro-based polymers because of their low cost of manufacturing, biocompatibility, ecofriendly and biodegradability. Lignin as the second richest and the only polyaromatics bio-polymer in plant which has been most studied for the numerous applications in different fields. But, in the past decade, the exploitation of lignin for the preparation of new smart materials with improved properties has been broadly sought, because lignin valorization plays one of the primary challenging issues of the pulp and paper industry and lignocellulosic biorefinery. Although, well suited chemical structure of lignin comprises of many functional hydrophilic and active groups, such as phenolic hydroxyls, carboxyls and methoxyls, which provides a great potential to be applied in the preparation of biodegradable hydrogels. In this review, lignin hydrogel is covered with preparation strategies, properties and applications. This review reports some important properties, such as mechanical, adhesive, self-healing, conductive, antibacterial and antifreezing properties were then discussed. Furthermore, herein also reviewed the current applications of lignin hydrogel, including dye adsorption, smart materials for stimuli sensitive, wearable electronics for biomedical applications and flexible supercapacitors. Overall, this review covers recent progresses regarding lignin-based hydrogel and constitutes a timely review of this promising material.

Porous Scaffolds Based on Polydopamine/Chondroitin Sulfate/Polyvinyl Alcohol Composite Hydrogels.

In this paper, porous scaffolds based on composite hydrogels were fabricated using polydopamine (PDA), chondroitin sulfate (CS), and polyvinyl alcohol (PVA) via the freezing/thawing method. Different characteristics of the prepared composite hydrogels, including the pore sizes, compression strength, lap shear strength, mass loss, and cytocompatibility were investigated. Scanning electron microscope images (SEM) displayed the hydrogel pore sizes, ranging from 20 to 100 µm. The composite hydrogel exhibited excellent porosity of 95.1%, compression strength of 5.2 MPa, lap shear strength of 21 kPa on porcine skin, and mass loss of 16.0%. In addition, the composite hydrogel possessed good relative cell activity of 97%. The PDA/CS/PVA hydrogel is cytocompatible as a starting point, and it can be further investigated in tissue engineering.

Plant-inspired conductive adhesive organohydrogel with extreme environmental tolerance as a wearable dressing for multifunctional sensors.

Conductive hydrogels have attracted significant attention as a promising material in electrical and biomedical fields. However, the simultaneous realization of good conductivity, toughness, high tissue adhesiveness, excellent biocompatibility, and extreme environmental tolerance remains a challenge. Inspired by the antifreezing/antiheating behavior of natural plants, a calcium chloride/TEMPO-oxidized cellulose nanofiber-dopamine/ polyacrylamide (CaCl2/TOCNF-DOPA/PAM) glycerol/water organohydrogel with antifreezing and antiheating properties, good transparency, conductivity, stability, excellent biocompatibility, mechanical properties, and tissue adhesiveness was fabricated. The organohydrogel has about 700% stretchability, with about 90% transparency. The organohydrogel exhibits good conductivity of 4.9 × 10-4 S/cm and high tissue adhesiveness of 50 kPa, which can monitor various human activities. The organohydrogel displays excellent extreme environmental tolerance to maintain the conductivity and mechanical properties under an extremely wide temperature range (-24 to 50 °C) for a long period due to its water-locking effect between glycerol and water molecules. The biocompatible organohydrogel is able to protect the skin from frostbite or burns in harsh environments. The plant-inspired stable and durable organohydrogel is used as a wearable dressing for multifunctional sensors.

A Green Catechol-Containing Cellulose Nanofibrils-Cross-Linked Adhesive.

Traditional adhesives with strong adhesion are widely applied in the fields of wood, building, and electronics. However, the synthesis and usage of commercial adhesives are not eco-friendly, which are harmful to human health and to the environment. In this study, a green cellulose nanofibrils/poly(hydroxyethyl methacrylate-co-dopamine methacrylamide) (CNFs/P(HEMA-co-DMA)) adhesive with excellent biocompatibility and strong bonding strength has been fabricated. P(HEMA-co-DMA) with a catechol content of 7.1 mol % was synthesized using dopamine methacrylamide and hydroxyethyl methacrylate. The CNFs/P(HEMA-co-DMA) adhesive was generated by cross-linking P(HEMA-co-DMA) solution using cellulose nanofibrils (CNFs). Strong adhesion was realized on various substrates, with a maximum lap shear strength of 5.50 MPa on steel. The NIH 3T3 cells test demonstrated that the adhesive possessed excellent biocompatibility. The green catechol-containing CNFs-cross-linked adhesive has promising potential for applications in medicine, electronic, food packaging, and engineering.

Mussel-inspired biocompatible polydopamine/carboxymethyl cellulose/polyacrylic acid adhesive hydrogels with UV-shielding capacity.

Hydrogels are attractive due to their various applications in the fields of biomedical materials, cosmetics, and biosensors. To enhance UV protection and prevent skin penetration behaviors, inspired by the mussel adhesive proteins, the functional polydopamine (PDA) is employed herein to fabricate polydopamine/carboxymethyl cellulose/polyacrylic acid (PDA/CMC/PAA) adhesive hydrogels. To disperse PDA nanoparticles well in the PAA matrix, dopamine was self-polymerized in CMC solution to form PDA/CMC complex. Acrylic acid was polymerized in PDA/CMC complex solution and cross-linked to construct UV-resistant PDA/CMC/PAA hydrogel. The morphology, rheological behavior, mechanical properties and adhesion strength of PDA/CMC/PAA hydrogels were studied by scanning electron microscopy, rotational rheometer, universal test machine. Owing to the hydrogen bonding interaction between the PDA/CMC complex and PAA, the PDA/CMC/PAA hydrogels showed high resilience and compressive strength to withstand large deformation. The hydrogels exhibited strong adhesion to various substrate surfaces, such as stainless steel, aluminum, glass and porcine skin. The biocompatibility and UV-shielding properties were investigated through culture of cells and UV irradiation test. The adhesiveness of PDA promoted cell adhesion and provided the PDA/CMC/PAA hydrogels good biocompatibility with 96% of relative cell viability. The hydrogels possessed excellent UV-shielding ability to prevent collagen fibers from being destroyed during UV irradiation, which has promising potential in the practical applications for UV filtration membrane and skin care products.

Mussel-inspired cellulose-based adhesive with biocompatibility and strong mechanical strength via metal coordination.

Inspired by marine mussel, catechol-containing materials, such as adhesives, self-healing hydrogels, and antifouling coatings, have been developed with wide applications in chemical, biomedical, and electronics industries. Conventionally, petrochemicals or organic solvents are widely used for preparation and dissolution of adhesives, which makes the adhesives are not eco-friendly and biocompatible. To develop environmentally friendly and biocompatible adhesives with desired properties, here we report catechol-containing cellulose-based tissue adhesives, synthesized by incorporating catechol groups onto cellulose. The structures of the adhesives with different catechol contents were analyzed by UV-vis spectroscopy, Fourier transform infrared spectroscopy (FTIR) and nuclear magnetic resonance (1H NMR) spectroscopy. The adhesion strengths were examined using porcine skin by lap shear tensile tests. The adhesion strength of the as-prepared adhesive with catechol content of 16.5 mol% was 20.0 kPa. Fe3+ was used as crosslinker to enhance the adhesion strength and accelerate the solidification of adhesives. Through the Fe3+-catechol coordination, the adhesion strength of adhesive was increased to 88.0 kPa, showing strong mechanical strength compared to the fibrin adhesive. NIH 3T3 cells test demonstrates that the adhesive is favorable for cell attachment and proliferation, possessing excellent biocompatibility. The catechol-containing cellulose-based adhesive has promising application in bioengineering field.

TEMPO-Oxidized Cellulose with High Degree of Oxidation.

In this paper, water-soluble 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose with a high degree of oxidation was prepared by a two-step process using bamboo dissolving pulp. The first step was to destroy the cellulose crystal I by NaOH/urea solution to obtain cellulose powder with decreased crystallinity. The second step was to oxidize the cellulose powder by TEMPO oxidation. The TEMPO-oxidized cellulose was analyzed by Fourier transform infrared spectroscopy (FTIR), conductimetry, X-ray diffraction (XRD), fiber analyzer, and transmission electron microscopy (TEM). FTIR showed that the hydroxymethyl groups in cellulose chains were converted into carboxyl groups. The degree of oxidation measured by conductimetry titration was as high as 91.0%. The TEMPO-oxidized cellulose was soluble in water for valuable polyelectrolytes and intermediates.