Advanced Applications of Porous Materials in Triboelectric Nanogenerator Self-Powered Sensors.

Porous materials possess advantages such as rich pore structures, a large surface area, low relative density, high specific strength, and good breathability. They have broad prospects in the development of a high-performance Triboelectric Nanogenerator (TENG) and self-powered sensing fields. This paper elaborates on the structural forms and construction methods of porous materials in existing TENG, including aerogels, foam sponges, electrospinning, 3D printing, and fabric structures. The research progress of porous materials in improving TENG performance is systematically summarized, with a focus on discussing design strategies of porous structures to enhance the TENG mechanical performance, frictional electrical performance, and environmental tolerance. The current applications of porous-material-based TENG in self-powered sensing such as pressure sensing, health monitoring, and human-machine interactions are introduced, and future development directions and challenges are discussed.

Mild Acetylation and Solubilization of Ground Whole Plant Cell Walls in EmimAc: A Method for Solution-State NMR in DMSO-d6.

Lignocellulosic biomass is mainly composed of polysaccharides and lignin. The complexity and diversity of the plant cell wall polymers makes it difficult to isolate the components in pure form for characterization. Many current approaches to analyzing the structure of lignocellulose, which involve sequential extraction and characterization of the resulting fractions, are time-consuming and labor-intensive. The present study describes a new and facile system for rationally derivatizing and dissolving coarsely ground plant cell wall materials. Using ionic liquids (EmimAc) and dichloroacetyl chloride as a solvent/reagent produced mildly acetylated whole cell walls without significant degradation. The acetylated products were soluble in DMSO-d6 from which they can be characterized by solution-state two-dimensional nuclear magnetic resonance (2D NMR) spectrometry. A distinct advantage of the procedure is that it realizes the dissolution of whole lignocellulosic materials without requiring harsh ball milling, thereby allowing the acquisition of high-resolution 2D NMR spectra to revealing structural details of the main components (lignin and polysaccharides). The method is therefore beneficial to understanding the composition and structure of biomass aimed at its improved utilization.

Predictors of Adoption and Reach Following Dialectical Behavior Therapy Intensive Training™.

Dialectical behavior therapy (DBT) is an evidence-based treatment for borderline personality disorder. The DBT Intensive Training™ is widely used to train community clinicians to deliver DBT, but little is known about its effectiveness. This study prospectively evaluated predictors of adoption and reach of DBT among 52 community teams (212 clinicians) after DBT Intensive Training™. Pre-post training questionnaires were completed by trainees and a follow-up survey by team leaders approximately 8 months later. Overall, 75% of teams adopted all DBT modes and delivered DBT to an average of 118 clients. Lower training and program needs, fewer bachelor's-level clinicians, and greater prior DBT experience predicted adoption of more DBT modes. More prior DBT experience, smaller team size, more negative team functioning, and staff with lower job satisfaction, growth, efficacy, and influence predicted greater DBT reach. DBT Intensive Training™ appears effective in promoting DBT adoption and reach in routine clinical practice settings.

EMT transcription factors activated circuits: A novel tool to study EMT dynamics and its therapeutic implications.

The epithelial mesenchymal transition (EMT) plays significant roles in the progression of cancer and fibrotic disease. Moreover, this process is reversible, resulting in mesenchymal epithelial transition (MET), which plays an important role in cancer metastasis. There is a lack of methods to trace and target EMT cells using synthetic biology circuits, which makes it difficult to study the cell fate or develop targeted treatments. In this study, we introduced responsive EMT sensing circuits, which sense the EMT using specific promoters that respond to transcription factors typical of EMT activation (EMT-TFs). The transcriptional strength of EMT-sensing promoters decreased more than 13-fold in response to the overexpression of the EMT-TF. Then, the NOT gate circuits were built by placing the tetR transcription repressor under the control of EMT sensing promoters and expressed an output signal using the constitutive CMV promoter modified with tetO sites This circuit is named EMT sensing and responding circuits .When the EMT transcription factors was present, we observed a 5.8-fold signal increase in the system. Then, we successfully distinguished mesenchymal breast cancer cells from epithelial cancer cells and repressed the proliferation of EMT tumor cells using our circuits. The EMT sensing and responding circuits are promising tools for the identification of EMT cells, which is crucial for EMT-related disease therapy and investigating the mechanisms underlying the reversible EMT process.

Facile dissolution of cellulose by superbase-derived ionic liquid using organic solvents as co-solvents at mild temperatures.

Dissolving cellulose at low temperatures is a key step in its efficient utilization as a renewable resource to produce high-value-added platform chemicals and high-performance materials. Here, the potential of four aprotic organic solvents was investigated for use as co-solvents with a sustainable DBU-derived ionic liquid (SIL) for the low-temperature dissolution and regeneration of cellulose. Combined experiments, density functional theory calculations, and molecular dynamic simulations were performed. The type and amount of co-solvent were found to have a significant impact on the solubility of cellulose, the dissolution process, and the structure of regenerated cellulose. The addition of organic solvents can significantly reduce the cellulose dissolution temperature and increase the solubility. Among the solvents assessed, 40 wt% DMSO exhibited the most effective synergistic interaction with SIL, where the solubility of cellulose was 14.6 wt% at 75 °C. Subsequently, the effects of the different types and amounts of co-solvents on the microscopic morphology and chemical structure of regenerated cellulose were thoroughly explored. The results showed that different types of organic solvents had different effects on the microstructure of regenerated cellulose. The results may guide the manufacturing specifications of high-performance regenerated fiber materials.

Preparation and characterization of cellulose-chitosan/ß-FeOOH composite hydrogels for adsorption and photocatalytic degradation of methyl orange.

Biopolymer-based hydrogels have received great attention in wastewater treatment due to their excellent properties, e.g., high adsorption capacity, fast kinetics, reusability and ease of operation. In the present work, cellulose-chitosan/ß-FeOOH composite hydrogels were prepared via co-dissolution and regeneration process as well as hydrothermal in situ synthesis of ß-FeOOH. Effect of ß-FeOOH loading on the properties of the composite hydrogels and the removal efficiency of methyl orange (MO) was investigated. Results showed that ß-FeOOH was uniformly loaded onto the hydrogel framework, and the nanoporous structure of composite hydrogels could increase not only the effective contact area between ß-FeOOH and the pollutants but also the active sites. Moreover, the increased ß-FeOOH loading led to the enhanced MO removal rate under light conditions. When the loading time was extended from 6 h to 9 h, the MO removal rate increased by 21%, which can be mainly due to the photocatalytic degradation. In addition, MO removal rate reached 97.75% within 40 min under optimal conditions and attained 80.81% after five repetitions. The trapping experiment and EPR results indicated that the main active species were hydrogel radicals and holes. Consequently, this work provides an effective preparation approach for cellulose-chitosan/ß-FeOOH composite hydrogel with high adsorption and photocatalytic degradation, which would hold great promise for wastewater treatment applications.

Synthesis and characterization of polyaniline-based composites using cellulose nanocrystals as biological templates.

Polyaniline (PANI) is considered as an ideal electrode material due to its remarkable Faradaic activity, exceptional conductivity, and ease of processing. However, the agglomeration and poor cycling stability of PANI largely limit its practical utilization in energy storage devices. To address these challenges, PANI was synthesized via a facile one-pot, two-step process using cellulose nanocrystals (CNCs) as bio-templates in this work. Zeta potential and particle size measurements revealed that the CNC template could impart improved dispersion stability to the synthesized PANI, which exhibited a decrease in average particle size from 1100 nm to 300 nm as a function of 10 % CNCs. Furthermore, the effect of CNC loadings on the performance of PANI was systematically investigated. The results showed that the specific capacitance of PANI/CNC increased from 102.52 F·g-1 to 138.12 F·g-1 with the CNC loading increase from 0 to 10 wt%. Particularly, the PANI/CNC composite film with a 1:9 ratio (C-P-10 %) demonstrated a capacity retention of 84.45 % after 6000 cycles and an outstanding conductivity of 526 S·m-1. This work generally offers an effective solution for the preparation of high-performance PANI-based composites, which might hold great promise in energy storage device applications.

Cellulose dissolution and regeneration behavior via DBU-levulinic acid solvents.

Most organic solvents are unable to dissolve carbohydrates due to the lack of hydrogen bonding ability. The development of solvent systems for dissolving cellulose is of great importance for its utilization and conversion. In this study, four new cellulose solvents were designed using inexpensive levulinic acid (LevA) and 1,8-diazabicyclo [5,4,0] undec-7-ene (DBU) as raw materials. The results showed that the prepared DBU-LevA-2 solvent was able to dissolve up to 7 wt% of bamboo cellulose (DP = 860) and 16 wt% of microcrystalline cellulose (DP = 280) at 100 °C and regenerated without derivatization. Also, the molar ratio of each component of this solvent has a significant effect on the dissolution properties of cellulose. The regenerated cellulose had the typical crystalline characteristics of cellulose II. Subsequently, the interactions and microscopic behaviors of solvent and cellulose during the dissolution process were thoroughly investigated by using NMR spectroscopy combined with density functional theory. The systematic study showed that the hydrogen bond-forming ability provided by DBU, a superbase, plays an indispensable role in the overall solvent system.

Facile synthesis of ZIF-8-lignosulfonate microspheres with ultra-high adsorption capacity for Congo red and tetracycline removal from water.

Zeolitic imidazolate frameworks (ZIFs) can be used as adsorbent to efficiently adsorb organic pollutants. However, the hydrophobicity of the ZIFs may be easily to form ZIFs nanoparticles aggregates, hampering the effective and practical application in adsorption. In this study, novel spherical composites of ZIF-8 incorporated with lignosulfonate (LS) were synthesized by in-situ growth method. The effects of different mass ratios of LS and Zn in ZIF-8-LS composites were evaluated with respect to structural characteristics and adsorption properties. As an adsorbent for adsorptive removing Congo Red (CR) and tetracycline (TC) from water, the prepared ZIF-8-LS4 shows the best adsorption capacity of 31.5 mg g-1 and 48 mg g-1, respectively. The spherical structure facilitates the contact between the ZIF-8 and the adsorbed substance, in addition to the H-bonding, electrostatic and π-π stacking interactions also contribute to the improvement of the adsorption performance of the ZIF-8-LS4 composite. The outstanding adsorption capacity and good reusability of the ZIF-8-LS4 composite provide a good prospect for the effective removal of other contaminants from water.

Highly Stretchable and Stimulus-Free Self-Healing Hydrogels with Multiple Signal Detection Performance for Self-Powered Wearable Temperature Sensors.

A flexible wearable temperature sensor is a novel electronic sensor that can monitor real-time changes in human body temperature in a variety of application scenarios and is regarded as the "crown jewel" of information collection technology. Although flexible strain sensors based on hydrogels have excellent self-healing effects and mechanical durability, their widespread application is still limited by external power sources. Herein, a novel self-energizing hydrogel was developed by embellishing cellulose nanocrystals (CNC) with poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS). The resultant thermoelectrically conductive CNC was then employed as a booster for poly(vinyl alcohol) (PVA)/borax hydrogels. The obtained hydrogels exhibit remarkable self-healing performance (92.57%) and exceptional stretchability (989.60%). Additionally, the hydrogel was capable of accurately and reliably identifying human motion. Most importantly, it exhibits excellent thermoelectric performance, capable of generating stable and reproducible voltages. It shows a large Seebeck coefficient of 1.31 mV k-1 at ambient temperatures. When subjected to a temperature difference of 25 K, the output voltage reaches 31.72 mV. CNC-PEDOT:PSS/PVA conductive hydrogel is multifunctional with self-healing, self-powering, and temperature sensing, which has the potential to be used for the preparation of intelligent wearable temperature-sensing devices.

Brain Registration and Evaluation for Zebrafish (BREEZE)-mapping: A pipeline for whole-brain structural and activity analyses.

Here, we present Brain Registration and Evaluation for Zebrafish (BREEZE)-mapping, a user-friendly pipeline for the registration and analysis of whole-brain images in larval zebrafish. We describe steps for pre-processing, registration, quantification, and visualization of whole-brain phenotypes in zebrafish mutants of genes associated with neurodevelopmental and neuropsychiatric disorders. By utilizing BioImage Suite Web, an open-source software package originally developed for processing human brain imaging data, we provide a highly accessible whole-brain mapping protocol developed for users with general computational proficiency. For complete details on the use and execution of this protocol, please refer to Weinschutz Mendes et al. (2023).1.

High-throughput functional analysis of autism genes in zebrafish identifies convergence in dopaminergic and neuroimmune pathways.

Advancing from gene discovery in autism spectrum disorders (ASDs) to the identification of biologically relevant mechanisms remains a central challenge. Here, we perform parallel in vivo functional analysis of 10 ASD genes at the behavioral, structural, and circuit levels in zebrafish mutants, revealing both unique and overlapping effects of gene loss of function. Whole-brain mapping identifies the forebrain and cerebellum as the most significant contributors to brain size differences, while regions involved in sensory-motor control, particularly dopaminergic regions, are associated with altered baseline brain activity. Finally, we show a global increase in microglia resulting from ASD gene loss of function in select mutants, implicating neuroimmune dysfunction as a key pathway relevant to ASD biology.

Cellulose nanofibril as a crosslinker to reinforce the sodium alginate/chitosan hydrogels.

Hydrogels derived from natural polymers have received great attention, but their practical applications are severely hindered by the relatively poor mechanical properties. In this work, cellulose nanofibril (CNF) was used as a crosslinker to reinforce the sodium alginate (SA)/chitosan (CS) hydrogels for drug sustained release. The CNF was prepared via a combined process of ball milling and deep eutectic solvents (DESs) pretreatment and characterized using SEM, FT-IR, and XRD. Furthermore, the microstructure, mechanical/biological properties and swelling performance of SA/CS/CNF hydrogels were investigated. Results showed that 1.0 wt% CNF addition led to the increases of 23.6% in storage modulus and 54.4% in loss modulus for the SA/CS/CNF hydrogels, indicating that CNF addition was effective in reinforcing the three-dimensional entangled networks of the hydrogels. Moreover, the presence of CNF was found to weaken the swelling performance of SA/CS/CNF hydrogels. When the synthesized SA/CS/CNF hydrogel with 1.0 wt% CNF was applied as a carrier for drug release, 50.8% reduction in the release rate in simulated gastric juice was achieved, demonstrating its outstanding sustained release properties. This work suggested that CNF might be conducive to enhancing the properties of SA/CS hydrogels, which can serve as an ideal polymeric carrier for drug release.

Spatial distribution and source of biotoxins in phytoplankton from the South China Sea, China.

Marine phycotoxins severely threaten ecosystem health and mariculture. This study investigates the spatial distribution and source of diverse phycotoxins in the South China Sea (SCS), during four 2019/2020 cruises. Saxitoxin (STX) and okadaic acid (OA) -groups, azaspiracids, cyclic imines, pectenotoxins (PTX), yessotoxins, and domoic acid (DA) toxins were analyzed in microalgal samples. PTX2 occurred with the highest (93.5%) detection rate (DR) during all cruises, especially in the Pearl River Estuary (PRE) in June 2019. Homo-yessotoxin (hYTX) and DA were found during three cruises in August 2020, and high DR of hYTX (67.7%, 29.3%) and DA (29.0%, 29.3%) in the PRE and Guangdong coast, respectively, in June 2019 and 2020, peaking at concentrations of 777 pg hYTX L-1 and 38514 pg DA L-1. The phycotoxin distribution demonstrated that DA-producing microalgae gathered close to the PRE and Guangdong coast, while hYTX-producing microalgae distributed relatively far offshore. Microalgae producing PTX2- and STX-group toxins were more widely living in the SCS. High-throughput sequencing results suggested that Alexandrium pacificum and Gonyaulax spinifera were responsible for STX-group toxins and hYTX, respectively, while Pseudo-nitzschia cuspidata was the main source of DA. Widely distributed PTX2, hYTX, and DA were reported for the first time in the SCS.

Synthesis of hemicellulose/deep eutectic solvent based carbon quantum dots for ultrasensitive detection of Ag+ and L-cysteine with "off-on" pattern.

The hypersensitive detection of metal ions and amino acid becomes more important for environmental and human physical conditions monitor but remains still a great challenge. In this work, we have reported a green and straight forward procedure (solvothermal treatment) for the synthesis of N-doped hemicellulose-based carbon quantum dots (N-H-CQDs) used as an "off-on" fluorescence sensor for ultrasensitive detecting Ag+ ion and L-Cysteine (L-Cys). During this process, hemicellulose used as carbon source and nitrogen-rich deep eutectic solvent (DES) of choline chloride/urea acted as both solvent and doping agent. The prepared N-H-CQDs displayed narrow diameter ranging from 2 to 8 nm with relatively higher quantum yield (QY) of 23.45%. This probe was able to selectively detect Ag+ ion on account of the formation of N-H-CQDs- Ag+ complex and possessed extremely low detection limit of 21 nM. Additionally, the fluorescence of N-H-CQDs-Ag+ complex was restored by the addition of L-Cysteine as Ag+ ion would assemble a more stable Ag+-L-Cysteine complex through Ag+-thiol bonds. Accordingly, the N-H-CQDs-Ag+ solution behaved as secondary fluorescent probe to detect L-Cys in the dynamic range of 0-100 µM with a LOD of 242 nM. The prepared N-H-CQDs are promising probes for hypersensitive detection of Ag+ and L-Cys.

Effects of Hydrothermal Pretreatment on the Structural Characteristics of Organosolv Lignin from Triarrhena lutarioriparia.

The effects of hydrothermal pretreatment (170⁻180 °C, 30⁻60 min) on the structural characteristics of enzymatic and extracted lignin from Triarrhena lutarioriparia (TL) during the integrated delignification process have been comprehensively investigated. Ion chromatography and NMR characterization showed that liquid products after mild hydrothermal process (170 °C, 30 min) were mainly composed of xylooligosaccharide (XOS) with different degrees of polymerization (DP ≥ 2). In addition, the structural changes of lignin during hydrothermal pretreatment and organic acid delignification process have been demonstrated by quantitative 2D heteronuclear single quantum coherence (2D-HSQC) and 31P-NMR techniques. Results showed that the structural changes of lignin (e.g., cleavage of ß-O-4 linkages) induced by the hydrothermal pretreatment will facilitate the subsequent organic acid delignification process, and acetylated lignin could be obtained with a considerable yield, which can be used in lignin-based composite and candidate feedstock for catalytic upgrading of lignin. In short, the proposed process facilitates the producing of XOS and acetylated lignin for lignin valorization.

Multi-analysis of chemical transformations of lignin macromolecules from waterlogged archaeological wood.

A large number of archaeological wooden building poles have been excavated from the Hai Menkou site (Yunnan province, China). Lignin can be transformed and altered accompanied with significant loss of carbohydrates during this process. Elucidation of chemical and structural transformations of lignin is of primary importance for understanding both the nature of degradation processes and the structure of waterlogged archaeological wood, and crucial for developing proper consolidation technology and restoring artifacts of historical and cultural value. In this study, state-of-the-art analytical techniques, including SEM, FT-IR, XRD, CP-MAS 13C NMR, 2D-HSQC NMR, 31P-NMR, CRM, GPC and TG analysis, were all employed to elucidate the structural characteristics of lignin in waterlogged and reference Pinus wood. The results interpreted by NMR analysis demonstrated the depolymerization of lignin via cleavage of ß-O-4, ß-5, -OCH3 and some LCC linkages, leading to a higher amount of free phenol OH groups in the lignin from the ancient waterlogged wood as compared to that of the reference wood. Microscopically, it was found that extensive degradation of carbohydrates in cell walls was mainly occurred in secondary cell walls, while the lignin concentrations were relatively increased in CCML and S regions in the plant cell wall of the ancient wood.

Amination of biorefinery technical lignins using Mannich reaction synergy with subcritical ethanol depolymerization.

The alcoholic depolymerization and Mannich reaction were conducted to improve the chemical activity of biorefinery technical lignins and introduce amino groups into lignins, respectively. To understand the chemical structural transformations and examine the reaction mechanism, GPC and solution-state NMR techniques were performed. Element analysis was also used to quantify the amount of amine groups. The NMR characterization the depolymerized lignins indicated of the depolymerization, demethoxylation, and bond cleavage of linkages occurred during the depolymerization process. Results showed that the depolymerization temperature instead of the addition of capping reagents was the main factor for improving the reactivity of lignin under the given conditions. The Mannich reaction was very selective, primarily occurred at H3,5 and G5 positions, and the H units present a higher chemical reactivity. It is believed that the understanding of the fundamental chemistry of lignin during depolymerization and Mannich reaction process will contribute to the extension of high value-added applications of biorefinery lignin.

Assessment of integrated process based on autohydrolysis and robust delignification process for enzymatic saccharification of bamboo.

In this study, bamboo (Phyllostachys pubescens) was successfully deconstructed using an integrated process (autohydrolysis and subsequent delignification). Xylooligosaccharides, high-purity lignin, and digestible substrates for producing glucose can be consecutively collected during the integrated process. The structural change and fate of lignin during autohydrolysis process was deeply investigated. Additionally, the structural characteristics and active functional groups of the lignin fractions obtained by these delignification processes were thoroughly investigated by NMR (2D-HSQC and 31P NMR) and GPC techniques. The chemical compositions (S, G, and H) and major linkages (ß-O-4, ß-ß, ß-5, etc.) were thoroughly assigned and the frequencies of the major lignin linkages were quantitatively compared. Considering the structural characteristics and molecular weights of the lignin as well as enzymatic saccharification ratio of the substrate, the combination of autohydrolysis and organic base-catalyzed ethanol pretreatment was deemed as a promising biorefinery mode in the future based on bamboo feedstock.

Structural variations of lignin macromolecule from different growth years of Triploid of Populus tomentosa Carr.

To better understand the variations of structural characteristics of lignin macromolecules during different growth years of Triploid of Populus tomentosa Carr, a novel lignin isolation procedure based on double ball-milling and enzymatic hydrolysis (DEL) was proposed in this study. The morphological distributions of lignin in the plant cell wall of these poplar wood samples were monitored by Confocal Raman Microscopy (CRM). The ultrahigh yields (105.1%-111.2%) of DELs were significantly higher than those (24.4-31.8%) of corresponding cellulolytic enzyme lignins (CELs). DELs and CELs were elaborately characterized by HPAEC, GPC, 2D-HSQC NMR and 31P NMR techniques, and NMR results showed that DEL samples possess similar structural features as compared to CEL counterparts except for the decreased S/G ratio and p-hydroxybenzoate (PB) as well as increased p-hydroxyphenyl units (H). There are no obvious differences in the structural characteristics except for high contents of PB and H units in DEL-1, as well as high S/G ratio and ß-O-4' linkages in DEL-5. It is believed that the DEL proposed in the present study can be used for characterizing the entire structural features of lignin macromolecules in the plant cell wall of different kinds of lignocellulosic biomass.