500 results on '"W Cai"'
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2. Strong Electrochemiluminescence Response Derived from Ionic Chiral Covalent Organic Frameworks for Enantioselective Discrimination of Amino Acid Enantiomers via an Electrostatic Attraction Effect.
- Author
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Yuan S, Cai W, Zhao L, Wang L, Zhang R, Li J, Wu D, and Kong Y
- Abstract
Porous chiral materials accompanied by electrochemiluminescence (ECL) activity are rarely reported for enantioselective discrimination because of the big challenges to integrate the stereogenic center and ECL-active unit in the backbone. In the present study, ionic chiral covalent organic frameworks (iCCOFs) consisting of the pyridinium unit as the ECL-active species were prepared by a facile strategy. We were amazed that such iCCOFs could display strong cathodic ECL responses. Meanwhile, the as-prepared ECL-active iCCOFs performed enantioselective ECL quenching toward amino acid enantiomers, attributed to the enhanced photoinduced electron transfer process derived from the formed complex between the iCCOFs and amino acids via an electrostatic attraction effect. The iCCOF with an ( S )-configuration was prone to interact with l-amino acids, producing a lower ECL intensity. The maximum intensity ratio between the d- and l-enantiomers was 33.0. Finally, the enantiomeric compositions of the measured amino acids presented a good linear relation with the obtained ECL intensity, which was fit for the determination of samples with unknown enantiomeric purity. In brief, the obtained results convince us that this study advances a new generation of ECL-active iCCOFs and displays great potential in enantioselective sensing.
- Published
- 2024
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3. Trop2-Targeted Molecular Imaging in Solid Tumors: Current Advances and Future Outlook.
- Author
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Liu Y, Huang W, Saladin RJ, Hsu JC, Cai W, and Kang L
- Abstract
Trophoblast cell surface antigen 2 (Trop2), a transmembrane glycoprotein, plays a dual role in physiological and pathological processes. In healthy tissues, Trop2 facilitates development and orchestrates intracellular calcium signaling. However, its overexpression in numerous solid tumors shifts its function toward driving cell proliferation and metastasis, thus leading to a poor prognosis. The clinical relevance of Trop2 is underscored by its utility as both a biomarker for diagnostic imaging and a target for therapy. Notably, the U.S. Food and Drug Administration (FDA) has approved sacituzumab govitecan (SG), a novel Trop2-targeted agent, for treating triple-negative breast cancer (TNBC) and refractory urothelial cancer, highlighting the significance of Trop2 in clinical oncology. Molecular imaging, a powerful tool for visualizing and quantifying biological phenomena at the molecular and cellular levels, has emerged as a critical technique for studying Trop2. This approach encompasses various modalities, including optical imaging, positron emission tomography (PET), single photon emission computed tomography (SPECT), and targeted antibodies labeled with radioactive isotopes. Incorporating Trop2-targeted molecular imaging into clinical practice is vital for the early detection, prognostic assessment, and treatment planning of a broad spectrum of solid tumors. Our review captures the latest progress in Trop2-targeted molecular imaging, focusing on both diagnostic and therapeutic applications across diverse tumor types, including lung, breast, gastric, pancreatic, prostate, and cervical cancers, as well as salivary gland carcinomas. We critically evaluate the current state by examining the relevant applications, diagnostic accuracy, therapeutic efficacy, and inherent limitations. Finally, we analyze the challenges impeding widespread clinical application and offer insights into strategies for advancing the field, thereby guiding future research endeavors.
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- 2024
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4. Electro-optically Modulated Nonlinear Metasurfaces.
- Author
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He Z, Qu L, Wu W, Liu J, Jin C, Wang C, You J, Liu W, Bai L, Gu Z, Cai W, Ren M, and Xu J
- Abstract
Electrically reconfigurable nonlinear metasurfaces provide dynamic control over nonlinear phenomena such as second-harmonic generation (SHG), unlocking novel applications in signal processing, light switching, and sensing. Previous methods, like electric-field-induced SHG in plasmonic metasurfaces and Stark-tuned nonlinearities in quantum well metasurfaces, face limitations due to weak SHG responses from metals and mid-infrared constraints of quantum wells, respectively. Addressing the need for efficient SHG control in the visible and near-infrared ranges, we present a novel approach using the electro-optic (EO) effect to modulate SHG. By leveraging the exceptional EO and SHG properties of lithium niobate (LN), we integrate the EO effect with SHG within a metasurface framework for the first time. Our LN metasurface achieves an 11.3% modulation depth in SHG amplitude under a ±50 V alternating voltage. These results open new avenues for reconfigurable photonic applications. including tunable nonlinear light sources, quantum optics, and nonlinear information processing.
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- 2024
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5. Immuno-PET Imaging of CD93 Expression with 64 Cu-Radiolabeled NOTA-mCD93 ([ 64 Cu]Cu-NOTA-mCD93) and Insulin-Like Growth Factor Binding Protein 7 ([ 64 Cu]Cu-NOTA-IGFBP7).
- Author
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Li X, Song W, Engle JW, Mixdorf JC, Barnhart TE, Sun Y, Zhu Y, and Cai W
- Abstract
CD93 is overexpressed in multiple solid tumor types, serving as a novel target for antiangiogenic therapy. The goal of this study was to develop a
64 Cu-based positron emission tomography (PET) tracer for noninvasive imaging of CD93 expression. Antimouse-CD93 mAb (mCD93) and the CD93 ligand IGFBP7 were conjugated to a bifunctional chelator, p -isothiocyanatobenzyl-1,4,7-triazacyclononane-1,4,7-triacetic acid ( p -SCN-NOTA) and labeled with64 Cu. To evaluate the pharmacokinetic properties and tumor-targeting efficacy of [64 Cu]Cu-NOTA-mCD93 and [64 Cu]Cu-NOTA-IGFBP7, PET imaging and biodistribution were performed on both 4T1 murine breast tumor-bearing mice and MDA-MB-231 human breast tumor-bearing mice. The tumor model HT1080-FAP, which does not overexpress CD93, was used as a negative control. Fluorescent immunostaining was conducted on different tissues to correlate radiotracer uptake with CD93 expression.64 Cu-labeling was achieved with high yield and specific activity. Serial PET imaging revealed that the in vivo performance of [64 Cu]Cu-NOTA-IGFBP7 was superior to that of [64 Cu]Cu-NOTA-mCD93, and that the tracer [64 Cu]Cu-NOTA-IGFBP7 exhibited elevated tumor uptake values and excellent tumor retention in MDA-MB-231 mice, rather than in 4T1 murine mice. The MDA-MB-231 tumor uptake of [64 Cu]Cu-NOTA-IGFBP7 was 2.85 ± 0.15, 3.69 ± 0.60, 6.91 ± 0.88, and 6.35 ± 0.55%ID/g at 1, 4, 24, and 48 h p.i., respectively, which were significantly higher than that in the CD93-negative HT1080-FAP tumor (0.73 ± 0.15, 0.97 ± 0.31, 1.00 ± 0.07, and 1.02 ± 0.11%ID/g, respectively). The significant difference between positive and negative tumors indicated [64 Cu]Cu-NOTA-IGFBP7 was specifically binding to CD93. Biodistribution data as measured by gamma counting were consistent with the PET analysis. Ex vivo histology further confirmed the high CD93 expression on MDA-MB-231 tumor tissues. Herein, we prepared two novel radiotracers, [64 Cu]Cu-NOTA-mCD93 and [64 Cu]Cu-NOTA-IGFBP7, for the first immune-PET imaging of CD93 expression. Our results suggest that [64 Cu]Cu-NOTA-IGFBP7 is a more potential radiotracer for visualizing angiogenesis due to its sensitive, persistent, and CD93-specific characteristics.- Published
- 2024
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6. Hierarchical Ordered Mesoporous Sr 2 Bi 4 Ti 5 O 18 Microflowers with Rich Oxygen Vacancies In Situ Assembled by Nanosheets for Piezo-Photocatalysis.
- Author
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Rao Z, Cai W, Yan Y, Huang R, Wang F, Wang Z, Gao R, Chen G, Deng X, Lei X, and Fu C
- Abstract
The Aurivillius phase layered perovskite ferroelectric material Sr
2 Bi4 Ti5 O18 (SBTO) exhibits spontaneous polarization and piezoelectric properties, which confer significant potential for piezo-photocatalysis. Its ability to enhance electron-hole separation while providing excellent fatigue resistance positions it as a promising candidate in this field. Defects were introduced to improve the structural polarization and photoelectrochemical properties of SBTO. SBTO nanocrystals, featuring a mixed structure of hierarchically ordered mesoporous microflowers and nanosheets, were successfully synthesized via the hydrothermal method. The SBTO sample synthesized at a lower hydrothermal temperature displayed optimal oxygen vacancy concentration and exhibited superior piezoelectric-photo synergistic degradation activity for organic pollutants. Additionally, corona polarization increases the macroscopic polarization of the SBTO photocatalyst, promoting the separation of photogenerated carriers. Finite element simulations confirmed that a single flower-like SBTO structure generates a higher piezoelectric potential compared to a sheet-like morphology. In conclusion, integrating self-assembled hierarchical structure design, ferroelectric polarization, and defect engineering forms an effective strategy for achieving high-performance SBTO-based layered perovskite piezo-photocatalysts.- Published
- 2024
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7. N-Terminal Capping of the αO-Conotoxin Analogue GeX-2 Improves the Serum Stability and Selectivity toward the Human α9α10 Nicotinic Acetylcholine Receptor.
- Author
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Li X, Zhou S, Tae HS, Wang S, Li T, Cai W, Jiang T, Adams DJ, and Yu R
- Subjects
- Humans, Animals, Rats, Male, Analgesics pharmacology, Analgesics chemistry, Analgesics chemical synthesis, Rats, Sprague-Dawley, Nicotinic Antagonists pharmacology, Nicotinic Antagonists chemistry, Nicotinic Antagonists chemical synthesis, Neuralgia drug therapy, Structure-Activity Relationship, Receptors, Nicotinic metabolism, Conotoxins chemistry, Conotoxins pharmacology, Conotoxins chemical synthesis
- Abstract
α9α10 nicotinic acetylcholine receptors (nAChRs) are a promising nonopioid analgesic target, with α9α10 nAChR antagonists showing efficacy against chemotherapy-induced hyperalgesia and allodynia. GeX-2, a potent analgesic conotoxin antagonist of α9α10 nAChRs, has limited serum stability. This study improved GeX-2 stability by capping its N-terminal with fatty acids or polyethylene glycol chains, which enhanced its serum stability but eliminated activity at G protein-coupled γ-aminobutyric acid type B (GABA
B ) receptor-coupled CaV 2.2 channels while preserving activity at α9α10 nAChRs. In vivo, α9α10 nAChRs antagonism alone did not alleviate neuropathic pain, highlighting the importance of GABAB receptor-coupled CaV 2.2 channels in GeX-2's antinociceptive effects in the chronic constriction injury rat model. The GeX-2 analogue, with an N-terminal methyl group, showed improved activity and selectivity for α9α10 nAChRs, increased serum half-life, and strong analgesic effects in oxaliplatin-induced cold allodynia models. AlphaFold3 and molecular dynamics simulations provided insights into the binding modes and the effects of N-terminal capping, which informed future peptide therapeutic developments.- Published
- 2024
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8. Abnormal Relaxation Behavior of Excited Electrons in the Flat Band of Kagome Compound Nb 3 Cl 8 .
- Author
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Meng Z, Shi Z, Feng H, Zhang H, Ren Z, Du Y, Cheng F, Ge B, Cai W, and Hao W
- Abstract
Carrier dynamics is crucial in semiconductors, and it determines their conductivity, response time, and overall functionality. In flat bands (FBs), carriers with high effective masses are predicted to host unconventional transport properties. The FBs usually overlap with other trivial energy bands, however, making it difficult to accurately distinguish their carrier dynamics. In this paper, we have investigated the flat-band carrier dynamics of excited electrons in Nb
3 Cl8 , which hosts ideal nonoverlapping FBs near the Fermi level. The optical transition between Hubbard bands is abnormally weakened, exhibiting weak interband absorption and its related slow photoresponse with a time constant of ∼120 s, which are associated with flat-band Mottness-induced large electron effective mass and parity-forbidden transitions. Besides, the localized states created by chlorine vacancies also act as trapping centers for carriers with a time constant of ∼600 s, which are similar to those of the compact localized states of the FB, making the relaxation behavior even more extraordinary. The presence and impacts of atomic defects are confirmed experimentally and theoretically. This work has revealed the abnormal flat-band carrier dynamics of Nb3 Cl8 , which is essential for understanding the optical, electrical, and thermal transport properties of flat-band materials.- Published
- 2024
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9. Optically Pure Co(III) Complex Absorbed by Electrochemiluminescence-Active Covalent Organic Framework as an Enantioselective Recognition Platform to Give Opposite Responses Toward Amino Alcohol Enantiomers.
- Author
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Zhao L, Cai W, Yuan S, Wang L, Zhang R, Li J, Wu D, and Kong Y
- Abstract
Although covalent organic frameworks (COFs) accompanied by electrochemiluminescence (ECL) behavior have been introduced in recent years, they are still rarely applied for ECL-based enantioselective sensing, especially giving high recognition efficiency. In the current study, an achiral ionic COF comprised of the pyridinium unit is synthesized in the linkage of the carbon-nitrogen cation bond through the Zincke reaction. Interestingly, the synthesized ionic COF can generate clear ECL owing to the presence of electroactive species. Then, the ECL-active achiral COF is employed to absorb the chiral Co(III) complex for enantioselective sensing. As a result, the developed ECL sensor displays discriminative responses toward amino alcohol enantiomers. When the chiral Co(III) complex with ( R )-configuration is used, the examined ( S )-amino alcohols result in ECL enhancement, whereas ( R )-amino alcohols lead to ECL quenching. The maximum ECL intensity ratio between ( S )- and ( R )-amino alcohols is up to 47.7. In addition, the recognition mechanism is investigated in detail. Finally, a good linear relation between enantiomeric composition and ECL intensity is developed and appropriate for the accurate analysis of the enantiomeric purities of unknown samples. In short, we believe that this study constructs an effective strategy to combine the respective advantages of COFs and ECL for high-efficiency enantioselective sensing.
- Published
- 2024
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10. Synthesis of P-Stereogenic Phosphinamides via Nickel-Catalyzed Kinetic Resolution of H-Phosphinamides by Alkenylation and Arylation.
- Author
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Xu C, Zhao J, Zheng Y, Cai W, and Wang C
- Abstract
A nickel-catalyzed enantioselective cross-coupling for the synthesis of P-stereogenic phosphinamides has been developed. The asymmetric alkenylation and arylation of racemic H-phosphinamides using alkenyl and aryl bromides resulted in the formation of P-stereogenic N-phosphinyl compounds with good yields and high enantioselectivities. This method tolerates a variety of functional groups, and its applications are explored through scale-up reactions and product transformations.
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- 2024
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11. Advances in Mussel Adhesion Proteins and Mussel-Inspired Material Electrospun Nanofibers for Their Application in Wound Repair.
- Author
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Dai Q, Liu H, Gao C, Sun W, Lu C, Zhang Y, Cai W, Qiao H, Jin A, Wang Y, and Liu Y
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- Animals, Humans, Proteins chemistry, Proteins metabolism, Biomimetic Materials chemistry, Biomimetic Materials pharmacology, Tissue Engineering methods, Biocompatible Materials chemistry, Biocompatible Materials pharmacology, Indoles, Polymers, Nanofibers chemistry, Wound Healing drug effects, Bivalvia chemistry
- Abstract
Mussel refers to a marine organism with strong adhesive properties, and it secretes mussel adhesion protein (MAP). The most vital feature of MAP is the abundance of the 3,4-dihydroxyphenylalanine (DOPA) group and lysine, which have antimicrobial, anti-inflammatory, antioxidant, and cell adhesion-promoting properties and can accelerate wound healing. Polydopamine (PDA) is currently the most widely used mussel-inspired material characterized by good adhesion, biocompatibility, and biodegradability. It can mediate various interactions to form functional coatings on cell-material surfaces. Nanofibers based on MAP and mussel-inspired materials have been exerting a vital role in wound repair, while there is no comprehensive review presenting them. This Review introduces the structure of MAPs and their adhesion mechanisms and mussel-inspired materials. Second, it introduces the functionalized modification of MAPs and their inspired materials in electrospun nanofibers and application in wound repair. Finally, the future development direction and coping strategies of MAP and mussel-inspired materials are discussed. Moreover, this Review can offer novel strategies for the application of nanofibers in wound repair and bring about new breakthroughs and innovations in tissue engineering and regenerative medicine.
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- 2024
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12. Overcoming Sampling Issues and Improving Computational Efficiency in Collective-Variable-Based Enhanced-Sampling Simulations: A Tutorial.
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Fu H, Zhou M, Chipot C, and Cai W
- Abstract
This tutorial is designed to help users overcome sampling challenges and improve computational efficiency in collective-variable (CV)-based enhanced-sampling, or importance-sampling, simulations. Toward this end, we introduce well-tempered metadynamics-extended adaptive biasing force (WTM-eABF) and its integration with Gaussian accelerated molecular dynamics (GaMD). Additionally, use will be made of a method for identifying the least-free-energy pathway (LFEP) and multiple concurrent pathways on high-dimensional free-energy surfaces. We illustrate these sampling techniques with the conformational equilibria of trialanine and chignolin in aqueous solution as test cases. This tutorial assumes that the user has prior experience with molecular dynamics (MD) simulations, in general, with the popular program NAMD, and to some extent with Colvars, the module for CV-based calculations. This tutorial can, however, in large measure be used in conjunction with alternate MD engines that support the Colvars module such as GROMACS, LAMMPS, and Tinker-HP.
- Published
- 2024
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13. Advances in Novel Biomaterial-Based Strategies for Spinal Cord Injury Treatment.
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Zhang N, Hu J, Liu W, Cai W, Xu Y, Wang X, Li S, and Ru B
- Subjects
- Humans, Animals, Nerve Regeneration drug effects, Spinal Cord Injuries therapy, Biocompatible Materials chemistry, Drug Delivery Systems methods
- Abstract
Spinal cord injury (SCI) is a highly disabling neurological disorder. Its pathological process comprises an initial acute injury phase (primary injury) and a secondary injury phase (subsequent chronic injury). Although surgical, drug, and cell therapies have made some progress in treating SCI, there is no exact therapeutic strategy for treating SCI and promoting nerve regeneration due to the complexity of the pathological SCI process. The development of novel drug delivery systems to treat SCI is expected to significantly impact the individualized treatment of SCI due to its unique and excellent properties, such as active targeting and controlled release. In this review, we first describe the pathological progression of the SCI response, including primary and secondary injuries. Next, we provide a concise overview of newly developed nanoplatforms and their potential application in regulating and treating different pathological processes of SCI. Then, we introduce the existing potential problems and future clinical application perspectives of biomedical engineering-based therapies for SCI.
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- 2024
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14. Ionic Covalent-Organic Frameworks Composed of Anthryl-Extended Viologen as a Kind of Electrochemiluminescence Luminophore.
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Zhang R, Cai W, Yuan S, Zhao L, Wang L, Li J, Wu D, and Kong Y
- Abstract
Nowadays, covalent-organic frameworks (COFs) integrated with the electrochemiluminescence (ECL) behavior are highly desired owing to the significant advantages including multifunctionality, high sensitivity, and low background noise. Here, two ionic COFs (iCOFs) consisting of the anthryl-extended viologen as the backbone were designed and synthesized via the Zincke reaction. It is found for the first time that the as-prepared iCOFs accompanied by potassium persulfate as the coreactant can provide a clear ECL response in a water-bearing medium. The maximum ECL emissions of the iCOFs were in agreement with the photoluminescence spectra. Besides, cyclic voltammetry and electron paramagnetic resonance measurements reveal that the pyridinium unit was electrochemically reduced to afford the free radical. Then, it reacted with SO
4 ·- to generate the excited-state [iCOF]*. Finally, [iCOF]* quickly returned to its ground state coupled with a clear ECL emission, yielding a maximum ECL quantum efficiency of 23.4% compared with tris(2,2'-bipyridyl) ruthenium(II) as the benchmark. In brief, the current study opens a way to develop a kind of ECL emitter that holds great potential in sensing, imaging, and light-emitting devices.- Published
- 2024
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15. Fluorine-Free Amphiphobic SBS/PAN Micro/Nanofiber Membrane by Integrating Click Reaction with Electrospinning for Efficient and Recyclable Air Filtration.
- Author
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Gou Y, Yang Y, Zheng W, Ji X, Lu N, Wang W, Zhong M, Shi Y, Huang J, Cai W, and Lai Y
- Subjects
- Filtration, Air Filters, Click Chemistry, Fluorine chemistry, Nanofibers chemistry, Membranes, Artificial
- Abstract
The membrane fouling derived from the accumulated dust pollutants and highly viscous oily particles causes irreversible damage to the filtration performance of air filters and results in a significant reduction in their service life. However, it is still challenging to construct high-efficiency and antifouling air filtration membranes with recyclable regeneration. Herein, the fluorine-free amphiphobic micro/nanofiber composite membrane was controllably constructed by integrating click chemistry reaction and electrospinning technique. Low-surface-energy fibers were constructed by a thiol-ene click chemical reaction between mercaptosilane and vinyl groups of polystyrene-butadiene-styrene (SBS), combined with hydroxyl-terminated poly(dimethylsiloxane) during the electrospinning process. The functional air filter is then prepared by the two-layer composite strategy. Because of the advantages of liquid-like fibrous surface and micro/nanofibrous porous structure, SBS/PAN composite membrane simultaneously shows superior antifouling performances of pollutants and filtration efficiency of over 97% PM
0.3 removal. More importantly, the antifouling fibrous membrane still presents a stable and efficient filtration efficiency after multiple washes. Its service life in dust filtration environments is approximately 1.7 times longer than that of the substrate membrane. This work may provide a significant reference for the design of antifouling fiber membranes and high-efficiency air filters with long life spans and reusability.- Published
- 2024
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16. Recycling of Spent Graphite from Lithium-Ion Batteries for Aqueous Zn Dual-Ion Batteries.
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Cai W, Zhang L, Chen K, Xiao M, Chen T, Dong X, Pu Z, Wan F, and Guo X
- Abstract
As lithium-ion batteries (LIBs) become more widespread, the number of spent LIBs gradually increases. Until now, recycling of spent LIBs has mainly concentrated on high-value cathodes, but the anode graphite has not yet attracted wide attention. In this work, spent graphite from LIBs was oxidized to graphene oxide and then thermally reduced to reduced graphene oxide (RGO), which serves as the cathode of aqueous Zn dual-ion batteries (ZDIBs). The thermal reduction process enables RGO with a large layer spacing and porous structure, which increase the anion insertion sites and transfer kinetics. As a result, the corresponding battery exhibits a high specific capacity of 96.82 mAh g
-1 at 1 A g-1 , superior rate capability, and a high capacity retention rate of 80% after 2000 cycles. Moreover, RGO gradually transforms into a long-range disordered structure during the cycling process, which provides more transport routes and active sites for anion insertion and thus leads to the increase of capacity. This work combines the recycling of spent graphite with aqueous ZDIBs, realizing the high-value use of spent graphite.- Published
- 2024
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17. Ultrahigh Transparent Safety Film for Spectrally Selective Photo/Electrothermal Conversion via Surface-Enhanced Plasma Resonance Dynamics.
- Author
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Cui T, Ang EH, Zheng Y, Cai W, Wang J, Hu Y, and Zhu J
- Abstract
Traditional deicing methods are increasingly insufficient for modern technologies like 5G infrastructure, photovoltaic systems, nearspace aerocraft, and terrestrial observatories. To address the challenge of combining anti-icing efficiency with operational performance, an innovative, spectrally selective, photo/electrothermic, ice-phobic film was prepared through a cost-effective mist deposition method. By manipulating the diameter ratio and density of nanowires, the local density of free electrons within this film is controlled to precisely dictate the position and intensity of surface plasmon resonance to achieve spectrally selective photo/electrothermal conversion. Additionally, the synthesized hydrophobic N-Boroxine-PDMS/SiO
2 layer improves thermal stability and accelerates the deicing process. It achieves rapid deicing within 86 s under photothermal conditions and 65 s with Joule heating while maintaining high optical transmittance. The film improves the operational efficiency and thermal safety of equipment while preserving aesthetics and stability, thereby underscoring its broad suitability for advanced outdoor installations in cold environments.- Published
- 2024
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18. Porous Spindle-Knot Fiber by Fiber-Microfluidic Phase Separation for Water Collection and Nanopatterning.
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Zou T, Ji Z, Cai W, Yang J, Wen G, Fu X, Yang W, and Wang Y
- Abstract
Porous spindle-knot structures have been found in many creatures, such as spider silk and the root of the soybean plant, which show interesting functions such as droplet collection or biotransformation. However, continuous fabrication of precisely controlled porous spindle-knots presents a big challenge, particularly in striking a balance among good structural controllability, low-cost, and functions. Here, we propose a concept of a fiber-microfluidics phase separation (FMF-PS) strategy to address the above challenge. This FMF-PS combines the advantages of a microchannel regulated Rayleigh instability of polymer solution coated onto a fiber with the nonsolvent-induced phase separation of the polymer solution, which enables continuous and cost-effective production of porous spindle-knot fiber (PSKF) with well-controlled size and porous structures. The critical factors controlling the geometry and the porous structures of the spindle-knot by FMF-PS have been systematically investigated. For applications, the PSKF exhibited faster water droplet nucleation, growth, and maximum water collection capability, compared to the control samples, as revealed by in situ water collection growth curves. Furthermore, high-level fabrics of the PSKFs, including a two-dimensional network and three-dimensional architecture, have been demonstrated for both large-scale water collection and art performance. Finally, the PSKF is demonstrated as a programmable building block for surface nanopatterning.
- Published
- 2024
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19. Biomimetic Colored Coating toward Robust Display under Hostile Conditions.
- Author
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Cheng Q, Chen J, Cai W, Yu X, Wan C, Wang Y, Xiong B, Huang C, and Yang Z
- Abstract
Structural colors particularly of the angle-independent category stemming from wavelength-dependent light scattering have aroused increasing interest due to their considerable applications spanning displays and sensors to detection. Nevertheless, these colors would be heavily altered and even disappear during practical applications, which is related with the variation of refractive index mismatch by liquid wetting/infiltrating. Inspired by bird feathers, we propose a simple deposition toward the coating with angle-independent structural color and superamphiphobicity. The coating is composed of ∼200 nm-sized channel-type structures between hollow silica and air nanostructures, exhibiting a robust sapphire blue color independent of intense liquid intrusion, which duplicates the characteristics of the back feather of Eastern Bluebird. A high color saturation and superamphiphobicity of the biomimetic coating are optimized by manipulating the coating parameters or adding black substances. Excellent durability under harsh conditions endows the coating with long-term service life in various extreme environments.
- Published
- 2024
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20. Catalyst-Free Domino Cross-Olefinations and Intramolecular Cyclizations of Morita-Baylis-Hillman Carbonates with Sulfur Ylides.
- Author
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Zhou Y, Cai W, and Huang Y
- Abstract
A novel strategy for the catalyst-free domino cross-olefination and intramolecular cyclization of Morita-Baylis-Hillman carbonates with sulfur ylides has been established, resulting in the synthesis of 1,2-dihydroquinolines with a broad scope, excellent chemoselectivity, and high efficiency. Mechanistic experiments revealed the process of 1,1-dipole cross-olefination and highlighted the assistance of the amino group in achieving successful transformations.
- Published
- 2024
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21. Pore-Specific Anisotropic Etching of Zeolitic Imidazolate Frameworks by Carboxylic Acid Vapors.
- Author
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Chen X, Cai W, Wang L, and Wang B
- Abstract
Anisotropic etching is a powerful way to customize metal-organic frameworks with advanced nanostructures, but it is still in its infancy. Herein, we proposed an unprecedented etching strategy that created anisotropic hollow structures in various zeolitic imidazolate framework (ZIF) nano/single crystals via pore-specific carving. The etching occurred through a newly discovered gas-solid reaction where carboxylic acid vapors bind with ligands in ZIFs at room temperature to form ionic liquid (IL). A series of experiments were conducted to decode the origin of anisotropy and the "hollowing out" effect. We found that large pore openings on {111} facets provide access for the entry of carboxylic acid vapors and the outflow of the IL, resulting in pore-dependent anisotropy features. The unique "etching after adsorption" mechanism and the adsorption capacity of the IL enable acid vapors to hollow out nanocrystals and even single crystals. By altering carboxylic acids and ligands in ZIFs, the etching process can be precisely tuned from the inside out or the outside in. This new method demonstrates broad universality and brings unprecedented morphologies and complexities. It may offer great opportunities for achieving purposeful modification of ZIFs and the rational construction of intricate architectures.
- Published
- 2024
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22. Fast In Vitro Synthesis and Direct Labeling of Nanobodies for Prototyping in Microscopy Applications.
- Author
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Behrens L, Walter RM, Cai W, Ewers H, van Bommel B, and Zemella A
- Abstract
Small antigen binders, such as nanobodies, have become widely used in biomedical research and pharmaceutical development. However, the pipeline for the generation of functional conjugated probes and drugs from identified binders remains a major time-consuming bottleneck. Here, we developed a method for fast nanobody production and conjugation based on an in vitro synthesis platform. Our system allows for small batch synthesis of nanobodies with the inclusion of a noncanonical amino acid (NCAA). This NCAA can then be used for direct conjugation of molecules to the synthesized nanobody using click-chemistry, reducing the time from binder-encoding DNA to a conjugated probe tremendously. In this study, we conjugated a fluorescent dye to an anti-Green fluorescent protein (GFP) nanobody and attained a fully functional probe suitable for advanced super-resolution microscopy within a short time frame of 2 days. Our work illustrates that an in vitro synthesis platform in combination with click-chemistry can be successfully employed to produce conjugated small antigen binding probes. The fast production and conjugation, combined with the possibility for parallelization as well as precise analysis by microscopy, forms an excellent platform for nanobody prototyping. The here-illustrated method can be used for quick selection and benchmarking of obtained nanobody sequences/clones, e. g., from a phage-display, for use as conjugated small-molecule carriers. This procedure can accelerate the bioengineering of nanobodies for research and pharmaceutical applications., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)
- Published
- 2024
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23. Enhanced Capability of Hydrogen Evolution Photocathode by Laminated Interface Engineering of Co/MoS 2 QDs/pyramid-black Si.
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Cai W, Gan Z, Nan F, Wang S, Ji F, and Zhan Y
- Abstract
We present a novel and stable laminated structure to enhance the performance and stability of silicon (Si) photocathode devices for photoelectrochemical (PEC) water splitting. First, by utilizing Cu nanoparticle catalysts to work on a n
+ p-black Si substrate via the metal-assisted chemical etching, we can achieve the black silicon with a porous pyramid structure. The low depth holes on the surface of the pyramid caused by Cu etching not only help enhance the light capture capability with quite low surface reflectivity (<5%) but also efficiently protect the p-n junction from damage. To improve the charge migration efficiency and mitigate parasitic light absorption from cocatalysts at the same time, we drop casted quantum dots (QDs) MoS2 with the size of nanometer scale as the first layer of catalyst. Hence, we then can safely electrodeposit cocatalyst Co nanoparticles to further enhance interface transfer efficiency. The synergistic effects of cocatalysts and optimized light absorption from the morphology and QDs contributed to the overall enhancement of PEC performance, offering a promising pathway for an efficient, low cost, and stable (over 100 h) hydrogen production photocathode.- Published
- 2024
- Full Text
- View/download PDF
24. AttenGpKa: A Universal Predictor of Solvation Acidity Using Graph Neural Network and Molecular Topology.
- Author
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An H, Liu X, Cai W, and Shao X
- Subjects
- Solubility, Hydrogen-Ion Concentration, Machine Learning, Models, Chemical, Acids chemistry, Solvents chemistry, Neural Networks, Computer
- Abstract
Rapid and accurate calculation of acid dissociation constant (p K
a ) is crucial for designing chemical synthesis routes, optimizing catalysts, and predicting chemical behavior. Despite recent progress in machine learning, predicting solvation acidity, especially in nonaqueous solvents, remains challenging due to limited experimental data. This challenge arises from treating experimental values in different solvents as distinct data domains and modeling them separately. In this work, we treat both the solutes and solvents equally from a perspective of molecular topology and propose a highly universal framework called AttenGpKa for predicting solvation acidity. AttenGpKa is trained using 26,522 experimental p Ka values from 60 pure and mixed solvents in the i BonD database. As a result, our model can simultaneously predict the p Ka values of a compound in various solvents, including pure water, pure nonaqueous, and mixed solvents. AttenGpKa achieves universality by using graph neural networks and attention mechanisms to learn complex effects within solute and solvent molecules. Furthermore, encodings of both solute and solvent molecules are adaptively fused to simulate the influence of the solvent on acid dissociation. AttenGpKa demonstrates robust generalization in extensive validations. The interpretability studies further indicate that our model has effectively learnt electronic and solvent effects. A free-to-use software is provided to facilitate the use of AttenGpKa for p Ka prediction.- Published
- 2024
- Full Text
- View/download PDF
25. Chirally Selective and Switchable Luminescence from Achiral Quantum Emitters on Suspended Twisted Stacking Metasurfaces.
- Author
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Cen M, Liu J, Wang J, Li Y, Cai W, Cheng M, Kong D, Tang X, Cao T, Lu YQ, and Liu YJ
- Abstract
Dynamic control of circularly polarized photoluminescence has aroused great interest in quantum optics and nanophotonics. Chiral plasmonic metasurfaces enable the manipulation of the polarization state via plasmon-photon coupling. However, current plasmonic light-emitting metasurfaces for effective deterministic modulation of spin-dependent emission at near-infrared wavelengths are underexplored in terms of dissymmetry and tunability. Here, we demonstrate a microfluidic hybrid emitting system of a suspended twisted stacking metasurface coated with PbS quantum dots. The suspended metasurface is fabricated with a single step of electron beam exposure, exhibiting a strong optical chirality of 309° μm
-1 with a thickness of less than λ/10 at key spectral locations. With significant chiral-selective interactions, enhanced photoluminescence is achieved with strong dissymmetry in circular polarization. The dissymmetry factor of the induced circularly polarized emission can reach 1.54. More importantly, altering the refractive index of the surrounding medium at the bottom surface of the metasurface can effectively manipulate the chiroptical responses of the hybrid system, hence leading to chirality-reversed emission. This active hybrid emitting system could be a resultful platform for chirality-switchable light emission from achiral quantum emitters, holding great potential for anticounterfeiting, biosensing, light sources, imaging, and displays.- Published
- 2024
- Full Text
- View/download PDF
26. Aluminum/Graphene Thermal Interface Materials with Positive Temperature Dependence.
- Author
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Cai W, Lu Y, Wang C, Li Q, and Zheng Y
- Abstract
Graphene is widely used in excellent thermal interface materials (TIMs), thanks to its remarkably high in-plane thermal conductivity ( k
∥ ). However, the poor through-plane thermal conductivity ( k of the 1.3-Al/GNPs composite to 11.70 W·m⊥ ) limits its further application. Here, we developed a simple in situ growth method to prepare graphene-based thermal interface composites with positively temperature-dependent thermal conductivity, which loaded aluminum (Al) nanoparticles onto graphene nanoplatelets (GNPs). To evaluate the variations in thermal performance, we determined the thermal diffusivity and specific heat capacity of the composites using a laser-flash analyzer and a differential scanning calorimeter, respectively. The Al nanoparticles act as bridges between the nanoplatelets, enhancing the k⊥ with temperature, reaching 20.93 W·m-1 ·K-1 at 25 °C. Even more remarkably, those nanoparticles led to a unique increase in k⊥ with temperature, reaching 20.93 W·m-1 ·K-1 at 100 °C. Additionally, we conducted an in-depth investigation of the thermal conductivity mechanism of the Al/GNPs composites. The exceptional heat transport property enabled the composites to exhibit a superior heat dissipation performance in simulated practical applications. This work provides valuable insights into utilizing graphene in composites with Al nanoparticles, which have special thermal conductivity properties, and offers a promising pathway to enhance the k⊥ of graphene-based TIMs.- Published
- 2024
- Full Text
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27. Design of Ultrasound-Driven Charge Interference Therapy for Wound Infection.
- Author
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Zhou J, Ji X, Wang H, Hsu JC, Hua C, Yang X, Liu Z, Guo H, Huang Y, Li Y, Cai W, Lin X, and Ni D
- Subjects
- Animals, Mice, Ultrasonic Waves, Reactive Oxygen Species metabolism, Wound Healing drug effects, Humans, Porphyrins chemistry, Porphyrins pharmacology, Porphyrins therapeutic use, Ultrasonic Therapy methods, Gram-Positive Bacteria drug effects, Gram-Negative Bacteria drug effects, Anti-Bacterial Agents pharmacology, Anti-Bacterial Agents chemistry, Anti-Bacterial Agents therapeutic use, Wound Infection drug therapy, Wound Infection microbiology, Nanoparticles chemistry, Nanoparticles therapeutic use, Biofilms drug effects
- Abstract
Wound infections, especially those caused by pathogenic bacteria, present a considerable public health concern due to associated complications and poor therapeutic outcomes. Herein, we developed antibacterial nanoparticles, namely, PGTP, by coordinating guanidine derivatives with a porphyrin-based sonosensitizer. The synthesized PGTP nanoparticles, characterized by their strong positive charge, effectively disrupted the bacterial biosynthesis process through charge interference, demonstrating efficacy against both Gram-negative and Gram-positive bacteria. Additionally, PGTP nanoparticles generated reactive oxygen species under ultrasound stimulation, resulting in the disruption of biofilm integrity and efficient elimination of pathogens. RNA-seq analysis unveiled the detailed mechanism of wound healing, revealing that PGTP nanoparticles, when coupled with ultrasound, impair bacterial metabolism by interfering with the synthesis and transcription of amino acids. This study presents a novel approach to combatting wound infections through ultrasound-driven charge-interfering therapy, facilitated by advanced antibacterial nanomaterials.
- Published
- 2024
- Full Text
- View/download PDF
28. Ginsenoside-Rh2 Promotes Functional Recovery after Spinal Cord Injury by Enhancing TFEB-Mediated Autophagy.
- Author
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Liu R, Jiang L, Chen Y, Shao J, Chen K, Li X, Lv J, Cai W, Cai H, Zhu Z, Wang C, Zhou K, Huang J, Xiao J, Ni W, and Wu C
- Subjects
- Animals, Mice, Humans, Mice, Inbred C57BL, Neuroprotective Agents pharmacology, Neuroprotective Agents administration & dosage, Male, Disease Models, Animal, Spinal Cord Injuries metabolism, Spinal Cord Injuries drug therapy, Spinal Cord Injuries physiopathology, Spinal Cord Injuries genetics, Ginsenosides pharmacology, Ginsenosides administration & dosage, Autophagy drug effects, Basic Helix-Loop-Helix Leucine Zipper Transcription Factors metabolism, Basic Helix-Loop-Helix Leucine Zipper Transcription Factors genetics, Recovery of Function drug effects
- Abstract
Background : Following spinal cord injury (SCI), autophagy plays a positive role in neuronal protection, whereas pyroptosis triggers an inflammatory response. Ginsenoside-Rh2 (GRh2), known for its neuroprotective effects, is considered a promising drug. However, the exact molecular mechanisms underlying these protective effects remain unclear. Aim of the Study : Explore the therapeutic value of GRh2 in SCI and its potential mechanisms of action. Materials and Methods : An SCI mouse model was established, followed by random grouping and drug treatments under different conditions. Subsequently, the functional recovery of SCI mice after GRh2 treatment was assessed using hematoxylin and eosin, Masson's trichrome, and Nissl staining, footprint analysis, Basso Mouse Scale scoring, and inclined plane tests. The expression levels of relevant indicators in the mice were detected using Western blotting, immunofluorescence, and a quantitative polymerase chain reaction. Network pharmacology analysis was used to identify the relevant signaling pathways through which GRh2 exerts its therapeutic effects. Results : GRh2 promoted functional recovery after SCI. GRh2 significantly inhibits pyroptosis by enhancing autophagy in SCI mice. Simultaneously, the neuroprotective effect of GRh2, achieved through the inhibition of pyroptosis, is partially reversed by 3-methyladenine, an autophagy inhibitor. Additionally, the increase in autophagy induced by GRh2 is mediated by the promotion of transcription factor EB (TFEB) nuclear translocation and dephosphorylation. Partial attenuation of the protective effects of GRh2 was observed after TFEB knockdown. Additionally, GRh2 can modulate the activity of TFEB in mice post-SCI through the EGFR-MAPK signaling pathway, and NSC228155 (an EGFR activator) can partially reverse the effect of GRh2 on the EGFR-MAPK signaling pathway. Conclusions : GRh2 improves functional recovery after SCI by upregulating TFEB-mediated autophagic flux and inhibiting pyroptosis, indicating its potential clinical applicability.
- Published
- 2024
- Full Text
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29. Monofluorophore-based Two-Photon Ratiometric Fluorescent Probe for the Quantitative Imaging of Fatty Acid Amide Hydrolase in Live Neurons and Mouse Brain Tissues.
- Author
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Gu X, Wang X, Cai W, Han Y, and Zhang QW
- Subjects
- Animals, Mice, Amyloid beta-Peptides metabolism, Amyloid beta-Peptides analysis, Humans, Pyridines chemistry, Alzheimer Disease metabolism, Alzheimer Disease diagnostic imaging, Photons, Amidohydrolases metabolism, Fluorescent Dyes chemistry, Fluorescent Dyes chemical synthesis, Brain diagnostic imaging, Brain metabolism, Neurons metabolism
- Abstract
Fatty acid amide hydrolase (FAAH) plays a crucial role in the metabolism of the endocannabinoid system by hydrolyzing a series of bioactive amides, whose abnormal levels are associated with neuronal disorders including Alzheimer's disease (AD). However, due to the lack of suitable quantitative sensing tools, real-time and accurate monitoring of the activity of FAAH in living systems remains unresolved. Herein, a novel enzyme-activated near-infrared two-photon ratiometric fluorescent probe (CANP) based on a naphthylvinylpyridine monofluorophore is successfully developed, in which the electron-withdrawing amide moiety is prone to be hydrolyzed to an electron-donating amine group under the catalysis of FAAH, leading to the activation of the intramolecular charge transfer process and the emergence of a new 80 nm red-shifted emission, thereby achieving a ratiometric luminescence response. Benefiting from the high selectivity, high sensitivity, and ratiometric response to FAAH, the probe CANP is successfully used to quantitatively monitor and image the FAAH levels in living neurons, by which an amyloid β (Aβ)-induced upregulation of endogenous FAAH activity is observed. Similar increases in FAAH activity are found in various brain regions of AD model mice, indicating a potential fatty acid amide metabolite-involved pathway for the pathological deterioration of AD. Moreover, our quantitative FAAH inhibition experiments further demonstrate the great value of CANP as an efficient visual probe for in situ and precise assessment of FAAH inhibitors in complex living systems, assisting the discovery of FAAH-related therapeutic agents.
- Published
- 2024
- Full Text
- View/download PDF
30. Responsive Liquid Crystal Network Microstructures with Customized Shapes and Predetermined Morphing for Adaptive Soft Micro-Optics.
- Author
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Cheng M, Cai W, Wang Z, Chen L, Yuan D, Ma Z, Bai Z, Kong D, Cen M, Xu S, Srivastava AK, and Liu YJ
- Abstract
Stimuli-responsive materials have garnered substantial interest in recent years, particularly liquid crystal networks (LCNs) with sophisticatedly designed structures and morphing capabilities. Extensive efforts have been devoted to LCN structural designs spanning from two-dimensional (2D) to three-dimensional (3D) configurations and their intricate morphing behaviors through designed alignment. However, achieving microscale structures and large-area preparation necessitates the development of novel techniques capable of facilely fabricating LCN microstructures with precise control over both overall shape and alignment, enabling a 3D-to-3D shape change. Herein, a simple and cost-effective in-cell soft lithography (ICSL) technique is proposed to create LCN microstructures with customized shapes and predesigned morphing. The ICSL technique involves two sequential steps: fabricating the desired microstructure as the template by using the photopolymerization-induced phase separation (PIPS) method and reproducing the LCN microstructures through templating. Meanwhile, surface anchoring is employed to design and achieve molecular alignment, accommodating different deformation modes. With the proposed ICSL technique, cylindrical and spherical microlens arrays (CMLAs and SMLAs) have been successfully fabricated with stimulus-driven polarization-dependent focusing effects. This technique offers distinct advantages including high customizability, large-area production, and cost-effectiveness, which pave a new avenue for extensive applications in different fields, exemplified by adaptive soft micro-optics and photonics.
- Published
- 2024
- Full Text
- View/download PDF
31. An Ultra-broadband Metallic Plasmonic Antenna for Ultrasensitive Molecular Fingerprint Identification.
- Author
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Zhong S, Guan Z, Yang F, Jiang Y, Zhao L, Wang W, Liu D, Cai W, and Li Y
- Abstract
Near-field enhanced mid-infrared light-matter interactions via metallic plasmonic antennae (PA) have attracted much attention but are inevitably limited by the detuning between their narrow band and the broad applied spectral range. Here, we develop a new low-temperature incubation synthetic method to acquire uniform Ag microparticles (MPs) with numerous hotspots. Their plasmonic band is remarkably extended by the plasmonic coupling of numerous hotspots and covers the entire mid-infrared range (400-4000 cm
-1 ). Hence, the almost complete molecular fingerprint of 4-mercaptobenzonitrile was successfully probed for the first time via resonant surface-enhanced infrared absorption (rSEIRA), and the rSEIRA spectra of different essential amino acids were further detected and exhibit a high spectral identification degree assisted by machine learning. This work changes the inertia perception of "narrow band and large size but small hotspot area" of mid-infrared metallic PA and paves the way for the ultrasensitive mid-infrared optical sensing.- Published
- 2024
- Full Text
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32. Integration of MoS 2 Memtransistor Devices and Analogue Circuits for Sensor Fusion in Autonomous Vehicle Target Localization.
- Author
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Tan T, Guo H, Li Y, Wang Y, Cai W, Bao W, Zhou P, and Feng X
- Abstract
In contemporary autonomous driving systems relying on sensor fusion, traditional digital processors encounter challenges associated with analogue-to-digital conversion and iterative vector-matrix operations, which are encumbered by limitations in terms of response time and energy consumption. In this study, we present an analogue Kalman filter circuit based on molybdenum disulfide (MoS
2 ) memtransistor, designed to accelerate sensor fusion for precise localization in autonomous vehicle applications. The nonvolatile memory characteristics of the memtransistor allow for the storage of a fixed Kalman gain, which eliminates the data convergence and thus accelerates the processing speeds. Additionally, the modulation of multiple conductance states by the gate terminal enables fast adaptability to diverse autonomous driving scenarios by tuning multiple Kalman filter gains. Our proposed analogue Kalman filter circuit accurately estimates the position coordinates of target vehicles by fusing sensor data from light detection and ranging (LiDAR), millimeter-wave radar (Radar), and camera, and it successfully solves real-word problems in a signal-free crossroad intersection. Notably, our system achieves a 1000-fold improvement in energy efficiency compared to that of digital circuits. This work underscores the viability of a memtransistor for achieving fast, energy-efficient real-time sensing, and continuous signal processing in advanced sensor fusion technology.- Published
- 2024
- Full Text
- View/download PDF
33. Phosphine-Catalyzed Domino Annulation of γ-Vinyl Allenoates: Synthesis of Tetrahydrofuro[3,2- c ]quinoline Derivatives.
- Author
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Ma M, Feng J, Cai W, and Huang Y
- Abstract
A novel phosphine-catalyzed domino annulation reaction of γ-vinyl allenoates and o -aminotrifluoacetophenones for the construction of terahydrofuro[3,2- c ]quinoline derivatives has been developed. In this domino reaction, two kinds of terahydrofuro[3,2- c ]quinoline compounds containing CF
3 groups were obtained with good yields under mild conditions, three new C-N, C-C, and C-O bonds can be built in one step, and the reaction selectivity is achieved by adjusting the reaction conditions. Furthermore, preliminary studies on an asymmetric variant of this reaction proceeded with moderate enantioselectivity.- Published
- 2024
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34. π-π + Interaction Promoting the Absorption of Electroactive Chiral Selectors into the Cavity of Conductive Covalent Organic Framework for Enantioselective Sensing of Electrochemically Silent Molecules.
- Author
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Wang F, Tan L, Li J, Cai W, Wu D, and Kong Y
- Abstract
To date, achieving enantioselective electroanalysis for electrochemically silent chiral molecules is still highly desired. Here, an ionic covalent organic framework (COF) consisting of the pyridinium cation was derived from the tripyridinium Zincke salt and 1,4-phenylenediamine in a one-pot reaction. The electrochemical measurements revealed that the ionic backbone contributed to the electron transfer with a low charge transfer resistance. Besides, the π-π
+ interaction between the pyridinium cation and ferrocenyl unit can promote the absorption of electroactive chiral ferrocenyl reagents into the hole of COF, so as to afford the electrochemical signals by themselves, replacing the testing enantiomers. As a result, the electroactive complex used as an electrochemical platform was highly effective at enantiomerically recognizing amino alcohols (prolinol, valinol, leucinol, and alaninol) and amino acids (methionine, serine, and penicillamine), giving the ratios of current intensity between l- and d-enantiomers in the range of 1.46-1.72. Moreover, the density functional theory calculations determined the possible intermolecular interactions between the testing enantiomers and chiral selector: namely, hydrogen bonds and electrostatic attractions. Overall, the present work offers an effective strategy to enlarge the electrochemical scope for chiral recognition based on electroactive chiral COFs.- Published
- 2024
- Full Text
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35. Construction of a Robust Radiative Cooling Emitter for Efficient Food Storage and Transportation.
- Author
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Tao S, Cai W, Han J, Shi C, Fang Z, Lu C, Xu C, Li W, and Xu Z
- Abstract
Nowadays, food safety is still facing great challenges. During storage and transportation, perishable goods have to be kept at a low temperature. However, the current logistics still lack enough preservation ability to maintain a low temperature in the whole. Hence, considering the temperature fluctuation in logistics, in this work, the passive radiative cooling (RC) technology was applied to package to enhance the temperature control capability in food storage and transportation. The RC emitter with selective infrared emission property was fabricated by a facile coating method, and Al
2 O3 was added to improve the wear resistance. The sunlight reflectance and infrared emittance within atmospheric conditions could reach up to 0.92 and 0.84, respectively. After abrasion, the sunlight reflection only decreased by 0.01, and the infrared emission showed a negligible change, revealing excellent wear resistance. During outdoor measurement, the box assembled by RC emitters (RC box) was proved to achieve temperature drops of ∼9 and ∼4 °C compared with the corrugated box and foam box, respectively. Besides, the fruits stored in the RC box exhibited a lower decay rate. Additionally, after printing with patterns to meet the aesthetic requirements, the RC emitter could also maintain the cooling ability. Given the superior optical properties, wear resistance, and cooling capability, the emitter has great potential for obtaining a better temperature control ability in food storage and transportation.- Published
- 2024
- Full Text
- View/download PDF
36. Understanding the Reversible Binding of a Multichain Protein-Protein Complex through Free-Energy Calculations.
- Author
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Bian H, Shao X, Cai W, and Fu H
- Subjects
- Entropy, Protein Binding, Thermodynamics, Insulin chemistry, Molecular Dynamics Simulation
- Abstract
We demonstrate that the binding affinity of a multichain protein-protein complex, insulin dimer, can be accurately predicted using a streamlined route of standard binding free-energy calculations. We find that chains A and C, which do not interact directly during binding, stabilize the insulin monomer structures and reduce the binding affinity of the two monomers, therefore enabling their reversible association. Notably, we confirm that although classical methods can estimate the binding affinity of the insulin dimer, conventional molecular dynamics, enhanced sampling algorithms, and classical geometrical routes of binding free-energy calculations may not fully capture certain aspects of the role played by the noninteracting chains in the binding dynamics. Therefore, this study not only elucidates the role of noninteracting chains in the reversible binding of the insulin dimer but also offers a methodological guide for investigating the reversible binding of multichain protein-protein complexes utilizing streamlined free-energy calculations.
- Published
- 2024
- Full Text
- View/download PDF
37. Flexible and Energy-Efficient Synaptic Transistor with Quasi-Linear Weight Update Protocol by Inkjet Printing of Orientated Polar-Electret/High- k Oxide Composite Dielectric.
- Author
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Li Y, Cai W, Tao R, Shuai W, Rao J, Chang C, Lu X, and Ning H
- Abstract
Inkjet printing artificial synapse is cost-effective but challenging in emulating synaptic dynamics with a sufficient number of effective weight states under ultralow voltage spiking operation. A synaptic transistor gated by inkjet-printed composite dielectric of polar-electret polyvinylpyrrolidone (PVP) and high- k zirconia oxide (ZrO
x ) is proposed and thus synthesized to solve this issue. Quasi - linear weight update with a large variation margin is obtained through the coupling effect and the facilitation of dipole orientation, which can be attributed to the orderly arranged molecule chains induced by the carefully designed microfluidic flows. Crucial features of biological synapses including long-term plasticity, spike-timing-dependence-plasticity (STDP), "Learning-Experience" behavior, and ultralow energy consumption (<10 fJ/pulse) are successfully implemented on the device. Simulation results exhibit an excellent image recognition accuracy (97.1%) after 15 training epochs, which is the highest for printed synaptic transistors. Moreover, the device sustained excellent endurance against bending tests with radius down to 8 mm. This work presents a very viable solution for constructing the futuristic flexible and low-cost neural systems.- Published
- 2024
- Full Text
- View/download PDF
38. Synergistically Optimized Thermoelectric and Mechanical Properties of Mg 3.2 Bi 1.5 Sb 0.5 -SiC Composites.
- Author
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Yu K, Dong X, Zhu Y, Zhang Y, Ge Z, Guo F, Cai W, Liu Z, and Sui J
- Abstract
Motivated by the surging demand for low-temperature waste heat harvesting, materials with both prominent thermoelectric and good mechanical properties are preferred in practical applications. In this present work, the composite exploration of Te-doped Mg
3.2 Bi1.5 Sb0.5 - x vol % nanosized SiC ( x = 0, 0.05, 0.1, 0.2, and 0.5) was carried out, where nanosized SiC is physically dispersed in the matrix in the form of a second phase. SiC second phase compositing further optimized the matrix carrier concentration, resulting in a higher power factor in the service temperature range (the highest value from 28.9 to 31.7 μW cm-1 K-2 ), and the (ZT)ave from 0.91 to 0.96 compared with the matrix sample. In addition, the SiC second phase effectively enhanced the mechanical properties of composite materials, including flexural strength, microhardness, and modulus. Because of the simultaneous optimization of thermoelectric and mechanical properties, the overall performance of Te-doped Mg3.2 Bi1.5 Sb0.5 -0.05 vol % SiC composite is leveraged to meet special requirements of power generation. It is expected that the addition of SiC should be broadly applicable to address the physical performance in other thermoelectric systems.- Published
- 2024
- Full Text
- View/download PDF
39. Projection of Mortality Burden Attributable to Nonoptimum Temperature with High Spatial Resolution in China.
- Author
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Yin P, He C, Chen R, Huang J, Luo Y, Gao X, Xu Y, Ji JS, Cai W, Wei Y, Li H, Zhou M, and Kan H
- Subjects
- Temperature, Cities, China epidemiology, Climate Change, Mortality, Cold Temperature, Hot Temperature
- Abstract
The updated climate models provide projections at a fine scale, allowing us to estimate health risks due to future warming after accounting for spatial heterogeneity. Here, we utilized an ensemble of high-resolution (25 km) climate simulations and nationwide mortality data from 306 Chinese cities to estimate death anomalies attributable to future warming. Historical estimation (1986-2014) reveals that about 15.5% [95% empirical confidence interval (eCI):13.1%, 17.6%] of deaths are attributable to nonoptimal temperature, of which heat and cold corresponded to attributable fractions of 4.1% (eCI:2.4%, 5.5%) and 11.4% (eCI:10.7%, 12.1%), respectively. Under three climate scenarios (SSP126, SSP245, and SSP585), the national average temperature was projected to increase by 1.45, 2.57, and 4.98 °C by the 2090s, respectively. The corresponding mortality fractions attributable to heat would be 6.5% (eCI:5.2%, 7.7%), 7.9% (eCI:6.3%, 9.4%), and 11.4% (eCI:9.2%, 13.3%). More than half of the attributable deaths due to future warming would occur in north China and cardiovascular mortality would increase more drastically than respiratory mortality. Our study shows that the increased heat-attributable mortality burden would outweigh the decreased cold-attributable burden even under a moderate climate change scenario across China. The results are helpful for national or local policymakers to better address the challenges of future warming.
- Published
- 2024
- Full Text
- View/download PDF
40. Ultrasensitive Biomimetic Skin with Multimodal and Photoelectric Dual-Signal Sensing.
- Author
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Gao H, Cai W, Li A, Du Y, Zhu JL, and Ye Z
- Abstract
Mimicking biological skin enabling direct, intelligent interaction between users and devices, multimodal sensing with optical/electrical (OE) output signals is urgently required. Owing to this, this work aims to logically design a stretchable OE biomimetic skin (OE skin), which can sensitively sense complex external stimuli of pressure, strain, temperature, and localization. The OE skin consists of elastic thin polymer-stabilized cholesteric liquid crystal films, an ion-conductive hydrogel layer, and an elastic protective membrane formed with thin polydimethylsiloxane. The as-designed OE skin exhibits customizable structural color on demand, good thermochromism, and excellent mechanochromism, with the ability to extend the full visible spectrum, a good linearity of over 0.99, fast response speed of 93 ms, and wide temperature range of 119 °C. In addition, the conduction resistance variation of ion-conductive hydrogel exhibits excellent sensing capabilities under pressure, stretch, and temperature, endowing a good linearity of 0.99998 (stretching from 0 to 150%) and high thermal sensitivity of 0.86% per °C. Such an outstanding OE skin provides design concepts for the development of multifunctional biomimetic skin used in human-machine interaction and can find wide applications in intelligent wearable devices and human-machine interactions.
- Published
- 2024
- Full Text
- View/download PDF
41. Explainable Graph Neural Networks with Data Augmentation for Predicting p K a of C-H Acids.
- Author
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An H, Liu X, Cai W, and Shao X
- Subjects
- Databases, Factual, Materials Science, Naphthalenesulfonates, Neural Networks, Computer, Drug Discovery, Electronics
- Abstract
The p K
a of C-H acids is an important parameter in the fields of organic synthesis, drug discovery, and materials science. However, the prediction of p Ka is still a great challenge due to the limit of experimental data and the lack of chemical insight. Here, a new model for predicting the p Ka values of C-H acids is proposed on the basis of graph neural networks (GNNs) and data augmentation. A message passing unit (MPU) was used to extract the topological and target-related information from the molecular graph data, and a readout layer was utilized to retrieve the information on the ionization site C atom. The retrieved information then was adopted to predict p Ka by a fully connected network. Furthermore, to increase the diversity of the training data, a knowledge-infused data augmentation technique was established by replacing the H atoms in a molecule with substituents exhibiting different electronic effects. The MPU was pretrained with the augmented data. The efficacy of data augmentation was confirmed by visualizing the distribution of compounds with different substituents and by classifying compounds. The explainability of the model was studied by examining the change of p Ka values when a specific atom was masked. This explainability was used to identify the key substituents for p Ka . The model was evaluated on two data sets from the i BonD database. Dataset1 includes the experimental p Ka values of C-H acids measured in DMSO, while dataset2 comprises the p Ka values measured in water. The results show that the knowledge-infused data augmentation technique greatly improves the predictive accuracy of the model, especially when the number of samples is small.- Published
- 2024
- Full Text
- View/download PDF
42. Interpretable Perturbator for Variable Selection in near-Infrared Spectral Analysis.
- Author
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Duan C, Liu X, Cai W, and Shao X
- Subjects
- Least-Squares Analysis, Spectroscopy, Near-Infrared methods
- Abstract
A perturbator was developed for variable selection in near-infrared (NIR) spectral analysis based on the perturbation strategy in deep learning for developing interpretation methods. A deep learning predictor was first constructed to predict the targets from the spectra in the training set. Then, taking the output of the predictor as a reference, the perturbator was trained to derive the perturbation-positive (P
+ ) and perturbation-negative (P- ) features from the spectra. Therefore, the weight (σ) of the perturbator layer can be a criterion to evaluate the importance of the variables in the spectra. Ranking the spectral variables by the criterion, the number of the variables used in the quantitative model can be obtained through cross-validation. Three NIR data sets were used to evaluate the proposed method. The root mean squared error was found to be comparable with or superior to that obtained by the commonly used methods. Moreover, the selected spectral variables are interpretable in identifying the key spectral features related to the prediction target. Therefore, the proposed method provides not only an effective tool for optimizing quantitative model, but also an efficient way for explaining spectra of multicomponent samples.- Published
- 2024
- Full Text
- View/download PDF
43. Biocompatible Metal-Free Perovskite Membranes for Wearable X-ray Detectors.
- Author
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Liu X, Cui Q, Li H, Wang S, Zhang Q, Huang W, Liu C, Cai W, Li T, Yang Z, Ma C, Ren L, Liu SF, and Zhao K
- Abstract
Halide perovskites are emerging as promising materials for X-ray detection owing to their compatibility with flexible fabrication, cost-effective solution processing, and exceptional carrier transport behaviors. However, the challenge of removing lead from high-performing perovskites, crucial for wearable electronics, while retaining their superior performance, persists. Here, we present for the first time a highly sensitive and robust flexible X-ray detector utilizing a biocompatible, metal-free perovskite, MDABCO-NH
4 I3 (MDABCO = methyl- N '-diazabicyclo[2.2.2]octonium). This wearable X-ray detector, based on a MDABCO-NH4 I3 thick membrane, exhibits remarkable properties including a large resistivity of 1.13 × 1011 Ω cm, a high mobility-lifetime product (μ-τ) of 1.64 × 10-4 cm2 V-1 , and spin Seebeck effect coefficient of 1.9 nV K-1 . We achieve a high sensitivity of 6521.6 ± 700 μC Gyair -1 cm-2 and a low detection limit of 77 nGyair s-1 , ranking among the highest for biocompatible X-ray detectors. Additionally, the device exhibits effective X-ray imaging at a low dose rate of 1.87 μGyair s-1 , which is approximately one-third of the dose rate used in regular medical diagnostics. Crucially, both the MDABCO-NH4 I3 thick membrane and the device showcase excellent mechanical robustness. These attributes render the flexible MDABCO-NH4 I3 thick membranes highly competitive for next-generation, high-performance, wearable X-ray detection applications.- Published
- 2024
- Full Text
- View/download PDF
44. Unraveling Spatially Dependent Hydrophilicity and Reactivity of Confined Carbocation Intermediates during Methanol Conversion over ZSM-5 Zeolite.
- Author
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Wang C, Zheng M, Hu M, Cai W, Chu Y, Wang Q, Xu J, and Deng F
- Abstract
Carbocations play a pivotal role as reactive intermediates in zeolite-catalyzed methanol-to-hydrocarbon (MTH) transformations. However, the interaction between carbocations and water vapor and its subsequent effects on catalytic performance remain poorly understood. Using micro-magnetic resonance imaging (μMRI) and solid-state NMR techniques, this work investigates the hydrophilic behavior of cyclopentenyl cations within ZSM-5 pores under vapor conditions. We show that the polar cationic center of cyclopentenyl cations readily initiates water nucleus formation through water molecule capture. This leads to an inhomogeneous water adsorption gradient along the axial positions of zeolite, correlating with the spatial distribution of carbocation concentrations. The adsorbed water promotes deprotonation and aromatization of cyclopentenyl cations, significantly enhancing the aromatic product selectivity in MTH catalysis. These results reveal the important influence of adsorbed water in modulating the carbocation reactivity within confined zeolite pores.
- Published
- 2024
- Full Text
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45. Orientin Promotes Antioxidant Capacity, Mitochondrial Biogenesis, and Fiber Transformation in Skeletal Muscles through the AMPK Pathway.
- Author
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Liu K, Li X, Liu Z, Ming X, Han B, Cai W, Yang X, Huang Z, Shi Z, Wu J, Hao B, and Chen X
- Subjects
- Humans, Mice, Animals, Antioxidants metabolism, Organelle Biogenesis, Muscle, Skeletal metabolism, Muscle Fibers, Skeletal metabolism, Muscle Fibers, Slow-Twitch metabolism, Flavonoids metabolism, AMP-Activated Protein Kinases metabolism, Sleep Apnea, Obstructive metabolism, Glucosides
- Abstract
The sleep-breathing condition obstructive sleep apnea (OSA) is characterized by repetitive upper airway collapse, which can exacerbate oxidative stress and free radical generation, thereby detrimentally impacting both motor and sensory nerve function and inducing muscular damage. OSA development is promoted by increasing proportions of fast-twitch muscle fibers in the genioglossus. Orientin, a water-soluble dietary C-glycosyl flavonoid with antioxidant properties, increased the expression of slow myosin heavy chain (MyHC) and signaling factors associated with AMP-activated protein kinase (AMPK) activation both in vivo and in vitro . Inhibiting AMPK signaling diminished the effects of orientin on slow MyHC, fast MyHC, and Sirt1 expression. Overall, orientin enhanced type I muscle fibers in the genioglossus, enhanced antioxidant capacity, increased mitochondrial biogenesis through AMPK signaling, and ultimately improved fatigue resistance in C2C12 myotubes and mouse genioglossus. These findings suggest that orientin may contribute to upper airway stability in patients with OSA, potentially preventing airway collapse.
- Published
- 2024
- Full Text
- View/download PDF
46. Multifunctional Bagasse Foam with Improved Thermal Insulation and Flame Retardancy by a Borax-Induced Self-Assembly and Ambient Pressure Drying Technique.
- Author
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Zhang X, Han L, Zhang H, Cai W, Wang X, Wang S, Gao Y, Liu X, Li Y, and Zhang S
- Abstract
Cellulose foams are considered an effective alternative to plastic foam, because of their advantages of low density, high porosity, low thermal conductivity, and renewable nature. However, they still suffer from complex processing, poor mechanical properties, and flammability. As an agricultural waste, bagasse is rich in cellulose, which has attracted much attention. Inspired by the fact that borate ions can effectively enhance the strength of plant tissue by their cross-linking with polysaccharides, the present work designs and fabricates a series of multifunctional bagasse foams with robust strength and improved thermal insulation and flame retardancy via a unique borax-induced self-assembly and atmospheric pressure drying route using bagasse as a raw material, borate as a cross-linking agent, and chitosan as an additive. As a result, the optimized foam exhibits a high porosity (93.5%), a high hydrophobic water contact angle (150.4°), a low thermal conductivity (63.4 mW/(m·K) at 25 °C), and an outstanding flame retardancy. The present study provides a novel and inspiring idea for large-scale production of cellulose foams through an environmentally friendly and cost-effective approach.
- Published
- 2024
- Full Text
- View/download PDF
47. Developments and Trends of Nanotechnology Application in Sepsis: A Comprehensive Review Based on Knowledge Visualization Analysis.
- Author
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Fu J, Cai W, Pan S, Chen L, Fang X, Shang Y, and Xu J
- Subjects
- Humans, Nanotechnology methods, Diagnostic Imaging, Nanostructures therapeutic use, Nanoparticles therapeutic use, Sepsis diagnosis, Sepsis therapy
- Abstract
Sepsis, a common life-threatening clinical condition, continues to have high morbidity and mortality rates, despite advancements in management. In response, significant research efforts have been directed toward developing effective strategies. Within this scope, nanotechnology has emerged as a particularly promising field, attracting significant interest for its potential to enhance disease diagnosis and treatment. While several reviews have highlighted the use of nanoparticles in sepsis, comprehensive studies that summarize and analyze the hotspots and research trends are lacking. To identify and further promote the development of nanotechnology in sepsis, a bibliometric analysis was conducted on the relevant literature, assessing research trends and hotspots in the application of nanomaterials for sepsis. Next, a comprehensive review of the subjectively recognized research hotspots in sepsis, including nanotechnology-enhanced biosensors and nanoscale imaging for sepsis diagnostics, and nanoplatforms designed for antimicrobial, immunomodulatory, and detoxification strategies in sepsis therapy, is elucidated, while the potential side effects and toxicity risks of these nanomaterials were discussed. Particular attention is given to biomimetic nanoparticles, which mimic the biological functions of source cells like erythrocytes, immune cells, and platelets to evade immune responses and effectively deliver therapeutic agents, demonstrating substantial translational potential. Finally, current challenges and future perspectives of nanotechnology applications in sepsis with a view to maximizing their great potential in the research of translational medicine are also discussed.
- Published
- 2024
- Full Text
- View/download PDF
48. New Insights into Identification, Distribution, and Health Benefits of Polyamines and Their Derivatives.
- Author
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Qiao J, Cai W, Wang K, Haubruge E, Dong J, El-Seedi HR, Xu X, and Zhang H
- Subjects
- Animals, Spermidine, Plants, Spermine, Polyamines, Tandem Mass Spectrometry
- Abstract
Polyamines and their derivatives are ubiquitously present in free or conjugated forms in various foods from animal, plant, and microbial origins. The current knowledge of free polyamines in foods and their contents is readily available; furthermore, conjugated polyamines generate considerable recent research interest due to their potential health benefits. The structural diversity of conjugated polyamines results in challenging their qualitative and quantitative analysis in food. Herein, we review and summarize the knowledge published on polyamines and their derivatives in foods, including their identification, sources, quantities, and health benefits. Particularly, facing the inherent challenges of isomer identification in conjugated polyamines, this paper provides a comprehensive overview of conjugated polyamines' structural characteristics, including the cleavage patterns and characteristic ion fragments of MS/MS for isomer identification. Free polyamines are present in all types of food, while conjugated polyamines are limited to plant-derived foods. Spermidine is renowned for antiaging properties, acclaimed as antiaging vitamins. Conjugated polyamines highlight their anti-inflammatory properties and have emerged as the mainstream drugs for antiprostatitis. This paper will likely help us gain better insight into polyamines and their derivatives to further develop functional foods and personalized nutraceuticals.
- Published
- 2024
- Full Text
- View/download PDF
49. Chiral Ru-Based Covalent Organic Frameworks as An Electrochemiluminescence-Active Platform for the Enantioselective Sensing of Amino Acids.
- Author
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Yuan S, Tan L, Zhao L, Wang F, Cai W, Li J, Wu D, and Kong Y
- Subjects
- Amino Acids, Luminescent Measurements methods, Stereoisomerism, Methionine, Electrochemical Techniques methods, Metal-Organic Frameworks, Biosensing Techniques methods
- Abstract
Although several studies related with the electrochemiluminescence (ECL) technique have been reported for chiral discrimination, it still has to face some limitations, namely, complex synthetic pathways and a relatively low recognition efficiency. Herein, this study introduces a facile strategy for the synthesis of ECL-active chiral covalent organic frameworks (COFs) employed as a chiral recognition platform. In this artificial structure, ruthenium(II) coordinated with the dipyridyl unit of the COF and enantiopure cyclohexane-1,2-diamine was harnessed as the ECL-active unit, which gave strong ECL emission in the presence of the coreactant reagent (K
2 S2 O8 ). When the as-prepared COF was used as a chiral ECL-active platform, clear discrimination was observed in the response of the ECL intensity toward l- and d-enantiomers of amino acids, including tryptophan, leucine, methionine, threonine, and histidine. The biggest ratio of the ECL intensity between different configurations was up to 1.75. More importantly, a good linear relationship between the enantiomeric composition and the ECL intensity was established, which was successfully employed to determine the unknown enantiomeric compositions of the real samples. In brief, we believe that the proposed ECL-based chiral platform provides an important reference for the determination of the configuration and enantiomeric compositions.- Published
- 2024
- Full Text
- View/download PDF
50. Postsynthetic Modification Strategy for Constructing Electrochemiluminescence-Active Chiral Covalent Organic Frameworks Performing Efficient Enantioselective Sensing.
- Author
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Tan L, Cai W, Wang F, Li J, Wu D, and Kong Y
- Abstract
Electrochemiluminescence (ECL), integrating the characteristics of electrochemistry and fluorescence, has the advantages of high sensitivity and low background. However, only a few studies have been reported for enantioselective sensing based on the ECL-active platform because of the huge challenges in constructing tunable chiral ECL luminophores. Here, we developed a facile strategy to design and prepare ECL-active chiral covalent organic frameworks (COFs) Ph-triPy
+ -( R )-Ru(II) for enantioselective sensing. In such an artificial structure, the ionic skeleton of COFs was beneficial to the electron transfer on the working electrode surface and the chiral Ru-ligand was used as the chiral ECL-active luminophore. It was found that Ph-triPy+ -( R )-Ru(II) coupled with sodium persulfate (Na2 S2 O8 ) as the coreactant exhibited obvious ECL signals. More importantly, a clear difference toward l- and d-enantiomers was observed in the response of the ECL intensity, resulting in a uniform recognition law. That is, for amino alcohols, d-enantiomers (1 mM) measured by Ph-triPy+ -( R )-Ru(II) showed a higher ECL intensity compared with l-enantiomers. Differently, amino acids (1 mM) gave an inverse recognition phenomenon. The ECL intensity ratios between l- and d-enantiomers (1 mM) are in the range of 1.25-1.94 for serine, aspartic acid, glutamic acid, valine, leucine, leucinol, and valinol. What is more interesting is that the ECL intensity was closely related to the concentration of l-amino alcohols and d-amino acids, whereas their inverse configurations remained unchanged. In a word, the present concept demonstrates a feasible direction toward chiral ECL-active COFs and their potential for efficient enantioselective sensing.- Published
- 2024
- Full Text
- View/download PDF
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