Nanolignin-containing cellulose nanofibrils (LCNF)-enabled multifunctional ratiometric fluorescent bio-nanocomposite films for food freshness monitoring.

Herein, the nanolignin-containing cellulose nanofibrils (LCNF)-enabled ratiometric fluorescent bio-nanocomposite film is developed. Interestingly, the inclusion of LCNF in the cellulose-based film enhances the detecting performance of food freshness, such as high sensitivity to biogenic amines (BAs) (limit of detection (LOD) of up to 1.83 ppm) and ultrahigh discernible fluorescence color difference (ΔE = 113.11). The underlying mechanisms are the fluorescence resonance energy transfer (FRET), π - π interaction, and cation - π interaction between LCNF and fluorescein isothiocyanate (FITC), as well as the increased hydrophobicity due to lignin, which increases the interactions of amines with FITC. Its color stability (up to 28 days) and mechanical property (49.4 Mpa) are simultaneously improved. Furthermore, a smartphone based detecting platform is developed to achieve access to food safety. This work presents a novel technology, which can have a great potential in the field of food packaging and safety.

Lignin: A multi-faceted role/function in 3D printing inks.

3D printing technology demonstrates significant potential for the rapid fabrication of tailored geometric structures. Nevertheless, the prevalent use of fossil-derived compositions in printable inks within the realm of 3D printing results in considerable environmental pollution and ecological consequences. Lignin, the second most abundant biomass source on earth, possesses attributes such as cost-effectiveness, renewability, biodegradability, and non-toxicity. Enriched with active functional groups including hydroxyl, carbonyl, carboxyl, and methyl, coupled with its rigid aromatic ring structure and inherent anti-oxidative and thermoplastic properties, lignin emerges as a promising candidate for formulating printable inks. This comprehensive review presents the utilization of lignin, either in conjunction with functional materials or through the modification of lignin derivatives, as the primary constituent (≥50 wt%) for formulating printable inks across photo-curing-based (SLA/DLP) and extrusion-based (DIW/FDM) printing technologies. Furthermore, lignin as an additive with multi-faceted roles/functions in 3D printing inks is explored. The effects of lignin on the properties of printing inks and printed objects are evaluated. Finally, this review outlines future perspectives, emphasizing key obstacles and potential opportunities for facilitating the high-value utilization of lignin in the realm of 3D printing.

Preparation of Activated Carbon-Reinforced Composite Beads Based on MnO2/MCM-41@Fe3O4 and Calcium Alginate for Efficient Removal of Tetracycline in Aqueous Solutions.

Tetracycline (TC) is a common antibiotic; when untreated TC enters the environment, it will cause a negative impact on the human body through the food chain. In the present study, MnO2/MCM-41@Fe3O4 (FeMnMCM) prepared using a hydrothermal and redox method and Camellia oleifera shell-activated carbon (COFAC) prepared through alkali activation were encapsulated using alginate (ALG) and calcium chloride as a cross-linking matrix to give the composite beads COFAC-FeMnMCM-ALG. The resultant COFAC-FeMnMCM-ALG composite beads were then carefully characterized, showing a high immobilization of MnO2/MCM-41@Fe3O4, with porous COFAC as an effective bioadsorbent for enriching the pollutants in the treated samples. These bead catalysts were subsequently applied to the oxidative degradation of TC in a Fenton oxidation system. Several parameters affecting the degradation were investigated, including the H2O2 concentration, catalyst dosage, initial TC concentration, and temperature. A very high catalytic activity towards the degradation of TC was demonstrated. The electron paramagnetic resonance (EPR) and quenching results showed that ·OH and ·O2- were generated in the system, with ·OH as the main radical species. In addition, the COFAC-FeMnMCM-ALG catalyst exhibited excellent recyclability/reusability. We conclude that the as-prepared COFAC-FeMnMCM-ALG composite beads, which integrate MnO2 and Fe3O4 with bioadsorbents, provide a new idea for the design of catalysts for advanced oxidation processes (AOPs) and have great potential in the Fenton oxidation system to degrade toxic pollutants.

Bioinspired construction of petal-like regenerated PVDF/cellulose fibers for efficient fog harvesting.

Water collection from atmospheric fog was deemed to be an efficient and sustainable strategy to defuse the freshwater scarcity crisis. Fog harvesting and trapping fibers, therefore, has aroused extensive interest due to their ease of preparation, weave, and use. However, the traditional fibers used in fog collector usually have a low fog collection capacity and efficiency because of their unreasonable morphology and structure design. Herein, we proposed a simple process to construct advanced fibers using a one-step wet spinning of hydrophobic polyvinylidene fluoride (PVDF) and hydrophilic cellulose mixture fiber for fog harvesting. The as-prepared fibers featured a petaloid structure and surface hydrophobic gradient, thus facilitating fog deposition, water droplet formation, and drainage. The unique longitudinal groove structure above enabled the hybrid fiber to achieve an excellent fog collection efficiency of 2750.26 mg/cm2/h per monofilament, which outstripped most of other fiber materials. When woven these fibers were in a longitudinal array network with an interval of 1 mm, and the fog collection efficiency can maintain at 10.30 L/m2/h. Therefore, this work provided a new strategy for further exploration of effective fog collection by cellulose-based fiber materials.

Biomimetic design of micro- and nano-wrinkle wood surface via coating reinforced with hyperbranched polymer grafted cellulose nanofibers for skin-tactile performance.

Inspired from human skin, micro- and nano-wrinkled wood surface with skin-tactile performance was designed and developed using a waterborne UV-curable polyurethane acrylate coating and cellulose nofibers (CNF). To further improve the properties, the CNF was diacetylated to D-CNF and further grafted with a hyperbranched polymer containing rich end amino groups (HB-CNF). The surface structure and chemical reactions were characterized, and the skin-tactile performance of the coating was comprehensively investigated. The HB-CNF exhibited excellent dispersion in the coating, and extensive reactions occurred between the two through the -NH2 and terminal -NCO groups, resulting in much improved mechanical properties and durability. Micro-wrinkles with a width of approximately 12-15 µm and a height of 8-14 µm were created, and nano-protrusions of wrinkles ranging from to 50-100 nm were obtained. The coated surface was hydrophobic and exhibited high resilience after compression, with a gloss of 3.3 GU at an incident angle of 60° and a static friction coefficient of 0.26, both of which were similar to those of human skin. The results presented an effective strategy for high-performance wood products with a good feeling, which is helpful to improve the market competitiveness and meet the people's pursuit of a better life.

Well-defined star (co)polypeptides via a fast, efficient, and metal-free strategy.

Polypeptides, especially star polypeptides, as a unique kind of biological macromolecules have broad applications in biomedical fields such as drug release, gene delivery, tissue engineering, and regenerative medicines due to their close structural similarity to naturally occurring peptides and proteins, biocompatibility, and amino acid functionality. However, the synthesis of star polypeptide mainly relies on the conventional primary amine-initiated ring-opening polymerization (ROP) of N-carboxyanhydrides (NCA) and suffers from low polymerization activity and limited controllability. This study proposes a fast, efficient and metal-free strategy to access star (co)polypeptides by combining the Michael reaction between acrylates and secondary aminoalcohols with the hydrogen-bonding organocatalytic ROP of NCA. This approach enables the preparation of a library of star (co)polypeptides with predesigned molecular weights, narrow molecular weight distributions, tunable arm number, and arm compositions. Importantly, this method exhibits high activity and selectivity at room temperature, making it both practical and versatile in synthesis applications.

Preparation of strong and tough conductive hydrogel based on Grafting, Fe3+-Catechol complexations and salting out for triboelectric nanogenerators.

The development of a strong and tough conductive hydrogel capable of meeting the strict requirements of the electrode of a hydrogel-based triboelectric nanogenerator (H-TENG) remains an enormous challenge. Herein, a robust conductive polyvinyl alcohol (PVA) hydrogel is designed via a three-step method: (1) grafting with 3,4-dihydroxy benzaldehyde, (2) metal complexation using ferric chloride (FeCl3) and (3) salting-out using sodium citrate. The hydrogel contains robust crystalline PVA domains and reversible/high-density non-covalent interactions, such as hydrogen bonding, π-π interactions and Fe3+-catechol complexations. Benefiting from the crystalline domains, the hydrogel can resist external forces to the hydrogel network; meanwhile, the reversible/high-density of non-covalent interactions can impart gradual and persistent energy dissipation during deformation. The hydrogel possesses multiple cross-linked networks, with 6.47 MPa tensile stress, 1000 % strain, 35.24 MJ/m3 toughness and 37.59 kJ/m2 fracture energy. Furthermore, the inter-connected porous hydrogel has an ideal structure for ionic-conducing channels. The hydrogel is assembled into an H-TENG, which can generate open circuit voltage of âˆ¼ 150 V, short-circuit current of âˆ¼ 3.0 µA, with superb damage immunity. Subsequently, road traffic monitoring systems are innovatively developed and demonstrated by using the H-TENG. This study provides a novel strategy to prepare superiorly strong and tough hydrogels that can meet the high demand for H-TENGs.

A novel process for efficient utilization of bamboo fiber resource in dissolving pulp production by fiber fractionation: Laboratory study and mill trials.

The rational use of bamboo to make dissolving pulp can offer up new opportunities for cellulose production, alleviating wood scarcity. Bamboo contains a high content of non-fiber cells, which presents technical challenges in dissolving pulp production by the conventional process. In this study, a process concept of separating hemicelluloses is presented by fiber fractionation and purification for cleaner production of bamboo dissolving pulp: bamboo kraft pulp was fractionated into long-fiber and short-fiber fractions. The cellulose-rich long-fiber fraction was converted to dissolving pulp by further purification treatment with acid hydrolysis and cold caustic extraction. The hemicellulose-rich short-fiber fraction was used for papermaking. The laboratory results were confirmed by those from mill trials. The combined pulp yield (dissolving pulp + paper-grade pulp) reached 49 %, which was significantly higher than that of the conventional pre-hydrolysis kraft pulping process. Furthermore, the quality of dissolving pulp was higher due to inherently higher cellulose content of long-fiber fraction.

Correction: Critical role of hydrogen bonding between microcrystalline cellulose and g-C3N4 enables highly efficient photocatalysis.

Correction for 'Critical role of hydrogen bonding between microcrystalline cellulose and g-C3N4 enables highly efficient photocatalysis' by Zhaoqiang Wang et al., Chem. Commun., 2024, 60, 204-207, https://doi.org/10.1039/D3CC04800D.

Promoting Electromagnetic Wave Absorption Performance by Integrating MoS2@Gd2O3/MXene Multiple Hetero-Interfaces in Wood-Derived Carbon Aerogels.

Multi-component composite materials with a magnetic-dielectric synergistic effect exhibit satisfactory electromagnetic wave absorption performance. However, the effective construction of the structure for these multi-component materials to fully exploit the advantages of each component remains a challenge. Inspired by natural biomass, this study utilizes wood as the raw material and successfully prepares high-performance MoS2@Gd2O3/Mxene loaded porous carbon aerogel (MGMCA) composite material through a one-pot hydrothermal method and carbonization treatment process. With a delicate structural design, the MGMCA is endowed with abundant heterogeneous interface structures, favorable impedance matching characteristics, and a magnetic-dielectric synergistic system, thus demonstrating multiple electromagnetic wave loss mechanisms. Benefiting from these advantages, the obtained MGMCA exhibits outstanding electromagnetic wave absorption performance, with a minimum reflection loss of -57.5 dB at an ultra-thin thickness of only 1.9 mm. This research proposes a reliable strategy for the design of multi-component composite materials, providing valuable insight for the design of biomass-based materials as electromagnetic wave absorbers.

Integrated Ink Printing Paper Based Self-Powered Electrochemical Multimodal Biosensing (IFP-Multi ) with ChatGPT-Bioelectronic Interface for Personalized Healthcare Management.

Personalized healthcare management is an emerging field that requires the development of environment-friendly, integrated, and electrochemical multimodal devices. In this study, the concept of integrated paper-based biosensors (IFP-Multi ) for personalized healthcare management is introduced. By leveraging ink printing technology and a ChatGPT-bioelectronic interface, these biosensors offer ultrahigh areal-specific capacitance (74633 mF cm-2 ), excellent mechanical properties, and multifunctional sensing and humidity power generation capabilities. More importantly, the IFP-Multi devices have the potential to simulate deaf-mute vocalization and can be integrated into wearable sensors to detect muscle contractions and bending motions. Moreover, they also enable monitoring of physiological signals from various body parts, such as the throat, nape, elbow, wrist, and knee, and successfully record sharp and repeatable signals generated by muscle contractions. In addition, the IFP-Multi devices demonstrate self-powered handwriting sensing and moisture power generation for sweat-sensing applications. As a proof-of-concept, a GPT 3.5 model-based fine-tuning and prediction pipeline that utilizes recorded physiological signals through IFP-Multi is showcased, enabling artificial intelligence with multimodal sensing capabilities for personalized healthcare management. This work presents a promising and ecofriendly approach to developing paper-based electrochemical multimodal devices, paving the way for a new era of healthcare advancements.

Critical role of hydrogen bonding between microcrystalline cellulose and g-C3N4 enables highly efficient photocatalysis.

Developing a highly efficient photocatalyst for energy and environmental applications is urgently required. Herein, graphitic carbon nitride (CN) coupled with microcrystalline cellulose (MCC) (denoted as MCC-X/CN) shows excellent photocatalytic performance for tetracycline (TC) degradation and H2 evolution. And the optimized MCC-0.05/CN shows an improved TC degradation rate (Kapp = 0.019 min-1) and H2 evolution rate (642.71 µmol g-1 h-1), which are 1.9 and 22 times higher than those of pure CN, respectively. This improvement primarily results from hydrogen bonding (H-bonding) between CN and MCC, which enables excellent charge separation and migration, leading to the outstanding photoelectrochemical properties of MCC-0.05/CN.

Multifunctional Conductive Material Based on Intelligent Porous Paper Used in Conjunction with a Vitrimer for Electromagnetic Shielding, Sensing, Joule Heating, and Antibacterial Properties.

With the continuous improvement of living standards and advancements in science and technology, composite materials with multiple functionalities are gaining high practical value in modern society. In this paper, we present a multifunctional conductive paper-based composite with electromagnetic (EMI) shielding, sensing, Joule heating, and antimicrobial properties. The composite is prepared by growing metallic silver nanoparticles inside the cellulose paper (CP) modified with polydopamine (PDA). The resulting CP@PDA@Ag (CPPA) composite has high conductivity and EMI shielding properties. Furthermore, CPPA composites demonstrate exceptional sensing, Joule heating, and antimicrobial properties. In addition, Vitrimer, a polymer with excellent cross-linked network structure, is introduced into CPPA composites to obtain CPPA-V intelligent electromagnetic shielding materials with shape memory function. These excellent properties show that the prepared multifunctional intelligent composite has exceptional EMI shielding, sensing, Joule heating, and antibacterial and shape memory properties. In short, this multifunctional intelligent composite material has great application prospects in flexible wearable electronics.

Preparation of a Novel Formaldehyde-Free Impregnated Decorative Paper Containing MnO2 Nanoparticles for Highly Efficient Formaldehyde Removal.

The loading of catalytic manganese dioxide (MnO2) nanoparticles onto an impregnated decorative paper has been an effective method for the removal of indoor formaldehyde (HCHO) pollutants. However, its preparation can present numerous challenges, including instability in dipping emulsions and leaching. In this investigation, a novel and stable formaldehyde-free polyacrylate dipping emulsion containing MnO2 particles was prepared and then back-coated on a decorative paper. To improve the dispersion and fixation, the MnO2 was modified with silane. HCHO can undergo physical adsorption on the cellulosic fibers present in the paper, while it can also undergo chemical degradation into CO2 within the MnO2 groups. The silane not only enhanced the interfacial adhesion to a polyacrylate resin but also increased the interlayer distance, thereby creating a larger space for HCHO absorption. The impregnated decorative paper back-coated with 10 wt % of silane-modified MnO2 exhibited a removal efficiency of approximately 90% for HCHO at 20 °C. The removal rate further improved to approximately 100% when the temperature was increased to 60 °C. Moreover, it is worth noting that the release of volatile organic compounds was exceptionally minimal. Additionally, the particleboard bonded with this impregnated decorative paper exhibited an extremely low emission of HCHO, with a value that approached 0 mg·L-1. Furthermore, the bonding strength of the surface remained unaffected. Therefore, this study provides a simple and eco-friendly method for effectively removing HCHO, which can enhance indoor air quality.

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.

Competitive Coordination-Oriented Monodispersed Cobalt Sites on a N-Rich Porous Carbon Microsphere Catalyst for High-Performance Zn-Air Batteries.

Metal/nitrogen-doped carbon single-atom catalysts (M-N-C SACs) show excellent catalytic performance with a maximum atom utilization and customizable tunable electronic structure. However, precisely modulating the M-Nx coordination in M-N-C SACs remains a grand challenge. Here, we used a N-rich nucleobase coordination self-assembly strategy to precisely regulate the dispersion of metal atoms by controlling the metal ratio. Meanwhile, the elimination of Zn during pyrolysis produced porous carbon microspheres with a specific surface area of up to 1151 m2 g-1, allowing maximum exposure of Co-N4 sites and facilitating charge transport in the oxygen reduction reaction (ORR) process. Thereby, the monodispersed cobalt sites (Co-N4) in N-rich (18.49 at%) porous carbon microspheres (CoSA/N-PCMS) displayed excellent ORR activity under alkaline conditions. Simultaneously, the Zn-air battery (ZAB) assembled with CoSA/N-PCMS outperformed Pt/C+RuO2-based ZABs in terms of power density and capacity, proving that they have good prospects for practical application.

Environmentally friendly strategy to access self-healable, reprocessable and recyclable chitin, chitosan, and sodium alginate based polysaccharide-vitrimer hybrid materials.

Natural polysaccharides show enviable advantages for preparation of sustainable hybrid materials. However, in most cases, complex chemical modifications of natural polysaccharides are required, which not only causes changes of the inherent properties of polysaccharides, but also increases the manufacturing costs of the final materials. Therefore, it is highly desired to develop efficient and low-cost ways to access polysaccharides-containing hybrid materials. In this work, we report the environmentally friendly preparation of a new kind of polysaccharide-based materials, called polysaccharide-vitrimer hybrid materials, for the first time. The vitrimer synthesis and hybridization with polysaccharides can be achieved via a convenient one-pot method in absence of solvent and catalyst. In addition, time-consuming and labor-intensive physical/chemical modifications of natural polysaccharides are completely avoided. The resultant hybrid materials show good mechanical performance (tensile toughness is up to 13.7 MJ/m3), high thermal stability (Td,max is up to 457 °C), fast self-healing ability (self-healing efficiency is up to 99 % within 20s at 80 °C) and excellent reprocessability and recyclability (at least three cycles). Especially, conductive polysaccharide-vitrimer hybrid materials could be readily prepared from the resultant materials, exhibiting novel applications as flexible sensors and electromagnetic shielding materials (the EMI SE is up to 24.93 dB).

Enzymatic treatment processes for the production of cellulose nanomaterials: A review.

Cellulose nanomaterials have attracted much attention in recent years because of their unique properties. Commercial or semi-commercial production of nanocellulose has been reported in recent years. Mechanical treatments for nanocellulose production are viable but highly energy-intensive. Chemical processes are well reported; however, these chemical processes are not only costly, but also cause environmental concerns and end-use related challenges. This review summarizes recent researches on enzymatic treatment of cellulose fibers for the production of cellulose nanomaterials, with focus on novel enzymatic processes with xylanase and lytic polysaccharide monooxygenases (LPMO) to enhance the efficacy of cellulase. Different enzymes are discussed, including endoglucanase, exoglucanase and xylanase, as well as LPMO, with emphasis on the accessibility and hydrolytic specificity of LPMO enzymes to cellulose fiber structures. LPMO acts in a synergistic way with cellulase to cause significant physical and chemical changes to the cellulose fiber cell-wall structures, which facilitate the nano-fibrillation of the fibers.

UV and IR dual light triggered cellulose-based invisible actuators with high sensitivity.

Actuators are widely used in bionic devices and soft robots, among which invisible actuators have some unique applications, including performing secret missions. In this paper, highly visible transparent cellulose-based UV-absorbing films were prepared by dissolving cellulose raw materials using N-methylmorpholine-N-oxide (NMMO) and using ZnO nanoparticles as UV absorbers. Furthermore, transparent actuator was fabricated by growing highly transparent and hydrophobic polytetrafluoroethylene (PTFE) film on regenerated cellulose (RC)-ZnO composite film. In addition to its sensitive response to Infrared (IR) light, the as-prepared actuator also shows a highly sensitive response to UV light, which is attributed to the strong absorption of UV light by ZnO NPs. Thanks to the drastic differences in adsorption capacity between the RC-ZnO and PTFE materials for water molecules, the asymmetrically- assembled actuator demonstrates extremely high sensitivity and excellent actuation performance, with a force density of 60.5, a maximum bending curvature of 3.0 cm-1, and a response time of below 8 s. Bionic bug, smart door and the arm of excavator made from the actuator all exhibit sensitive responses to UV and IR lights.

Rational design of pyrrolic-N dominated carbon material derived from aminated lignin for Zn-ion supercapacitors.

Developing highly efficient, sustainable carbon cathodes is essential for emerging Zn-ion hybrid supercapacitors (ZICs). Herein, lignin's novel chemical modification (amination) has been developed to produce high quantity pyrrolic-N moieties as active sites. Furthermore, chemically modified amine moieties in lignin are vital as a natural self-activating template to generate hierarchical porosity in the 2D (graphene-like) architecture with exceedingly high surface area (2926.4 m2g-1). The rationally introduced dominated pyrrolic-N moieties boost the Zn-ion storage capacity and reaction kinetics due to the dual energy storage mechanism and efficient charge transfer between pyrrolic-N and Zn+2 ions. Furthermore, the pyrrolic-N species are energetically favorable for the adsorption of Zn+2 ions by the formation of N-Zn+2 chemical bonds. Besides, the nitrogen oxides reduce the intrinsic resistance and induce a more polarized surface, resulting in high wettability and efficient transfer of electrolytes into the pores of hydrophobic carbon materials. Subsequently, the chemically modified lignin-derived activated carbon material (Chem-ACM) as a cathode in ZICs delivers a high capacity of 161.2 mA h g-1 at 1 A g-1 with the admirable energy density of 106.7 W h kg-1 at 897 W kg-1 and excellent retention capacity (94%) after 10,000 cycles. Mainly, the assembled quasi solid-state ZICs using Chem-ACM retains the remarkable storage capacity (202 mA h g-1 at 0.2 Ag-1) even at a high bending angle. Notably, the Chem-ACM has been further employed in symmetric supercapacitors as an electrode, and it displays exceptional specific capacitance of 354 Fg-1 at 0.5 Ag-1 with tremendous energy (43.5 W h kg-1) and the power density (0.53 kW kg-1). Additionally, the charge storage capability of Chem-ACM is positively dependent on high nitrogen contents, and it is extrapolated that pyrrolic-N moieties are dominant active sites. Hence, the designed amination-assisted biocarbon synthesis provides a new way to prepare high nitrogen-containing biocarbon for ZICs and further understand pyrrolic-N species' impact on Zn-ion storage.