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ACS Applied Materials & Interfaces Jul 2024Hydrogels, as flexible materials, have been widely used in the field of flexible sensors. Human sweat contains a variety of biomarkers that can reflect the physiological...
Hydrogels, as flexible materials, have been widely used in the field of flexible sensors. Human sweat contains a variety of biomarkers that can reflect the physiological state of the human body. Therefore, it is of great practical significance and application value to realize the detection of sweat composition and combine it with human motion sensing through a hydrogel. Based on mussel-inspired chemistry, polydopamine (PDA) and gold nanoparticles (AuNPs) were coated on the surface of cellulose nanocrystals (CNCs) to obtain CNC-based nanocomposites (CNCs@PDA-Au), which could simultaneously enhance the mechanical, electrochemical, and self-healing properties of hydrogels. The CNCs@PDA-Au was composited with poly(vinyl alcohol) (PVA) hydrogel to obtain the nanocomposite hydrogel (PVA/CNCs@PDA-Au) by freeze-thaw cycles. The PVA/CNCs@PDA-Au has excellent mechanical strength (7.2 MPa) and self-healing properties (88.3%). The motion sensors designed with PVA/CNCs@PDA-Au exhibited a fast response time (122.9 ms), wide strain sensing range (0-600.0%), excellent stability, and fatigue resistance. With the unique electrochemical redox properties of uric acid, the designed hydrogel sensor successfully realized the detection of uric acid in sweat with a wide detection range (1.0-100.0 μmol/L) and low detection limit (0.42 μmol/L). In this study, the dual detection of human motion and uric acid in sweat was successfully realized by the designed PVA/CNCs@PDA-Au nanocomposite hydrogel.
PubMed: 38958653
DOI: 10.1021/acsami.4c07717 -
ACS Applied Materials & Interfaces Jul 2024Polyacrylonitrile (PAN) is an important commercial polymer, bearing atactic stereochemistry resulting from nonselective radical polymerization. As such, an accurate,...
Polyacrylonitrile (PAN) is an important commercial polymer, bearing atactic stereochemistry resulting from nonselective radical polymerization. As such, an accurate, fundamental understanding of governing interactions among PAN molecular units is indispensable for advancing the design principles of final products at reduced processability costs. While molecular dynamics (AIMD) simulations can provide the necessary accuracy for treating key interactions in polar polymers, such as dipole-dipole interactions and hydrogen bonding, and analyzing their influence on the molecular orientation, their implementation is limited to small molecules only. Herein, we show that the neural network interatomic potentials (NNIPs) that are trained on the small-scale AIMD data (acquired for oligomers) can be efficiently employed to examine the structures and properties at large scales (polymers). NNIP provides critical insight into intra- and interchain hydrogen-bonding and dipolar correlations and accurately predicts the amorphous bulk PAN structure validated by modeling the experimental X-ray structure factor. Furthermore, the NNIP-predicted PAN properties, such as density and elastic modulus, are in good agreement with their experimental values. Overall, the trend in the elastic modulus is found to correlate strongly with the PAN structural orientations encoded in the Hermans orientation factor. This study enables the ability to predict the structure-property relations for PAN and analogues with sustainable accuracy across scales.
PubMed: 38958640
DOI: 10.1021/acsami.4c04491 -
ACS Applied Materials & Interfaces Jul 2024Isoporous membranes produced from diblock copolymers commonly display a poor mechanical property that shows many negative impacts on their separation application. It is...
Isoporous membranes produced from diblock copolymers commonly display a poor mechanical property that shows many negative impacts on their separation application. It is theoretically predicted that dense films produced from symmetric triblock copolymers show much stronger mechanical properties than those of homologous diblock copolymers. However, to the best of our knowledge, symmetric triblock copolymers have rarely been fabricated into isoporous membranes before, and a full understanding of separation as well as mechanical properties of membranes prepared from triblock copolymers and homologous diblock copolymers has not been conducted, either. In this work, a cleavable symmetric triblock copolymer with polystyrene as the side block and poly(4-vinylpyridine) (P4VP) as the middle block was synthesized and designed by the RAFT polymerization using the symmetric chain transfer agent, which located at the center of polymer chains and could be removed to produce homologous diblock copolymers with half-length while having the same composition as that found in triblock copolymers. The self-assembly of these two copolymers in thin films and casting solutions was first investigated, observing that they displayed similar self-organized structures under these two conditions. When fabricated into isoporous membranes, they showed similar pore sizes (5-7% difference) and comparable rejection performance (∼10% difference). However, isoporous membranes produced from triblock copolymers showed significantly improved mechanical strength and higher toughness (2-10 times larger) as evidenced by the compacting resistance, strain-stress determination, and nanoindentation testing, suggesting the unique and novel structure-performance relationship in the isoporous membranes produced from symmetric triblock copolymers. The above finding will guide the way to fabricate mechanically robust isoporous membranes without notably changing the separation performance from rarely used symmetric triblock copolymers, which can be synthesized by the controlled polymerization as facilely as that found for diblock copolymers.
PubMed: 38958638
DOI: 10.1021/acsami.4c07113 -
The Biochemical Journal Jul 2024Filamin A is an essential protein in the cell cytoskeleton because of its actin binding properties and unique homodimer rod-shaped structure, which organises actin into... (Review)
Review
Filamin A is an essential protein in the cell cytoskeleton because of its actin binding properties and unique homodimer rod-shaped structure, which organises actin into three-dimensional orthogonal networks imperative to cell motility, spreading and adhesion. Filamin A is subject to extensive posttranslational modification (PTM) which serves to co-ordinate cellular architecture and to modulate its large protein-protein interaction network which is key to the protein's role as a cellular signalling hub. Characterised PTMs include phosphorylation, irreversible cleavage, ubiquitin mediated degradation, hydroxylation and O-GlcNAcylation, with preliminary evidence of tyrosylation, carbonylation and acetylation. Each modification and its relation to filamin A function will be described here. These modifications are often aberrantly applied in a range of diseases including, but not limited to, cancer, cardiovascular disease and neurological disease and we discuss the concept of target specific PTMs with novel therapeutic modalities. In summary, our review represents a topical 'one-stop-shop' that enables understanding of filamin A function in cell homeostasis and provides insight into how a variety of modifications add an extra level of Filamin A control.
Topics: Filamins; Humans; Protein Processing, Post-Translational; Animals; Phosphorylation; Neoplasms
PubMed: 38958472
DOI: 10.1042/BCJ20240121 -
Angewandte Chemie (International Ed. in... Jul 2024Rapidly synthesizing high-quality two-dimensional covalent organic frameworks (2D COFs) is crucial to their practical applications. Here, we use a machine-learning...
Rapidly synthesizing high-quality two-dimensional covalent organic frameworks (2D COFs) is crucial to their practical applications. Here, we use a machine-learning approach that overcomes the challenges associated with bottom-up model derivation for the non-classical 2D COF crystallization processes. The resulting model, referred to as NEgen1, establishes correlations among the induction time, nucleation rate, growth rate, bond-forming rate constants, and common solution synthesis conditions for 2D COFs that grow by a nucleation-elongation mechanism. The results elucidate the detailed competition between the nucleation and growth dynamics in solution, which has been inappropriately described previously by classical, empirical models with assumptions invalid for 2D COF polymerization. By understanding the dynamic processes at play, the NEgen1 model reveals a simple strategy of gradually increasing monomer addition speed for growing large 2D COF crystals. This insight enables us to rapidly synthesize large COF-5 colloids, which could only be achieved previously by prolonged reaction times or by introducing chemical modulators. These results highlight the potential for systematically improving the crystal quality of 2D COFs, which has wide-reaching relevance for many of the applications for which 2D COFs are speculated to be valuable.
PubMed: 38958453
DOI: 10.1002/anie.202408937 -
Angewandte Chemie (International Ed. in... Jul 2024Synthetic molecular photoswitches have taken center stage as high-precision tools to introduce light-responsiveness at the smallest scales. Today they are found in all...
Synthetic molecular photoswitches have taken center stage as high-precision tools to introduce light-responsiveness at the smallest scales. Today they are found in all areas of applied chemistry, covering materials research, chemical biology, catalysis, or nanotechnology. For a next step of applicability truly orthogonal photoswitching is highly desirable but to date such independent addressability of different photoswitches remains to be highly challenging. In this work we present the first example of all-visible, all-light responsive, and path independent orthogonal photoswitching. By combining two recently developed indigoid photoswitches - peri-anthracenethioindigo and a rhodanine-based chromophore - a four-state system is established and each state can be accessed in high yields completely independently and also with visible light irradiation only. The four states give rise to four different colors, which can be transferred to a solid polymer matrix yielding a versatile multi-state photochromic material. Further, combination with a fluorescent dye as third component is possible, demonstrating applicability of this orthogonal photoswitching system in all-photonic molecular logic behavior and information processing.
PubMed: 38958439
DOI: 10.1002/anie.202409214 -
Langmuir : the ACS Journal of Surfaces... Jul 2024Magnesium-based biodegradable metal bone implants exhibit superior mechanical properties compared to biodegradable polymers for orthopedic and cardiovascular stents. In...
Magnesium-based biodegradable metal bone implants exhibit superior mechanical properties compared to biodegradable polymers for orthopedic and cardiovascular stents. In this study, MgZZC-x (x = 1, 1.2) alloys were screened by in vitro biocompatibility tests in three simulated body fluids under nontoxic conditions. The MgZZC-1 alloys with better biocompatibility were selected to predict the days required for complete degradation. The evolution of degradation products was analyzed, and the mechanism of formation of the product film was inferred. A degradation kinetic model was established to investigate the effect of MEM components on the degradation of the alloys. The results demonstrate that the proteins in MEM can greatly retard the degradation progress by attaching to the surface of MgZZC-1 alloys, which are predicted to degrade completely within 341 days. The carbonate and phosphate buffers were adjusted to pH in MEM solution, delaying the degradation of magnesium alloys. This process in MEM more accurately reflects the actual degradation in the body and is superior to that in Hanks and SBF solutions. This study will promote the application of biodegradable materials in clinical medicine.
PubMed: 38958429
DOI: 10.1021/acs.langmuir.4c01715 -
ACS Applied Materials & Interfaces Jul 2024MnO/polypyrrole (PPy) composite films were deposited on fluorine-doped tin oxide (FTO) conductive glasses by a two-step wet-chemical method, including electrochemical...
MnO/polypyrrole (PPy) composite films were deposited on fluorine-doped tin oxide (FTO) conductive glasses by a two-step wet-chemical method, including electrochemical deposition and chemical bath deposition (CBD). The porous MnO films were first grown on FTO glasses by an electrodeposition method. Second, polypyrrole nanoparticles were polymerized by the oxidation-reduction reaction between MnO and pyrrole, using the presynthesized MnO as the skeleton. Then, MnO/PPy composite films with coral-like structures were obtained. The electrochemical and electrochromic (EC) properties of the prepared films were investigated. The results show that, compared to the single MnO or PPy film, the MnO/PPy composite film has a larger optical modulation (67.3% at a wavelength of 900 nm), faster response times (4 s for coloration and 3 s for bleaching), and a higher coloration efficiency (218.16 cm·C). The high coloration efficiency attests to the exceptional performance of the composite film in converting electrical signals into vivid color changes. The electrochemical stability test results show that the composite film maintains a stable EC performance after 200 coloration/bleaching cycles. The coral-like structures of the composite film are responsible for the better EC properties.
PubMed: 38958414
DOI: 10.1021/acsami.4c05669 -
Acta Cirurgica Brasileira 2024To evaluate using a biocellulose-based hydrogel as an adjuvant in the healing process of arterial ulcers.
PURPOSE
To evaluate using a biocellulose-based hydrogel as an adjuvant in the healing process of arterial ulcers.
METHODS
A prospective single group quasi-experimental study was carried out with chronic lower limb arterial ulcer patients. These patients received biocellulose-based hydrogel dressings and outpatient guidance on dressing and periodic reassessments. The primary outcomes were the ulcer-healing rate and product safety, which were assessed by ulcer area measured in photographic records of pre-treatment and posttreatment after 7, 30, and 60 days. Secondary outcomes were related to clinical assessment by the quality-of-life scores (SF-36 and EQ-5D) and pain, evaluated by the visual analogue scale (VAS).
RESULTS
Seventeen participants were included, and one of them was excluded. Six patients (37%) had complete wound healing, and all patients had a significant reduction in the ulcer area during follow-up (233.6mm2 versus 2.7mm2) and reduction on the score PUSH 3.0 (p < 0.0001). The analysis of the SF-36 and EQ-5D questionnaires showed a statistically significant improvement in almost all parameters analyzed and with a reduction of pain assessed by the VAS.
CONCLUSIONS
The biocellulose-based hydrogel was safe and showed a good perspective to promoting the necessary conditions to facilitate partial or complete healing of chronic arterial ulcers within a 60-day follow-up. Quality of life and pain were positively affected by the treatment.
Topics: Humans; Male; Female; Wound Healing; Prospective Studies; Middle Aged; Aged; Quality of Life; Treatment Outcome; Chronic Disease; Cellulose; Leg Ulcer; Bandages; Aged, 80 and over; Pain Measurement; Hydrogels
PubMed: 38958305
DOI: 10.1590/acb392924 -
ACS Applied Materials & Interfaces Jul 2024Gel electrolytes are a promising research direction due to their high safety. However, its poor room temperature conductivity along with complex preparation process...
Gel electrolytes are a promising research direction due to their high safety. However, its poor room temperature conductivity along with complex preparation process hinder its practical application. In this article, a type of zwitterionic gel electrolyte is prepared by in situ polymerization. The introduction of charged but nonmigrating zwitterionic copolymer in the polymer chain is beneficial to the dissociation of the lithium salt, improving the ion transport of the electrolyte on this account. At room temperature, the conductivity of lithium ion reaches 9.1 × 10 S cm, which contributes to achieve excellent electrochemical performance at high rates. The assembled Li|LiFePO cell also shows a capacity retention rate of 90.5% after 150 cycles at 0.5 C at room temperature as well as remarkable cycle stability at 1 C. These offer a novel tactic for the efficient and safe commercial application of lithium-ion batteries.
PubMed: 38958244
DOI: 10.1021/acsami.4c05762