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1.
J Chem Phys ; 160(21)2024 Jun 07.
Artículo en Inglés | MEDLINE | ID: mdl-38832730

RESUMEN

It is highly demanded to understand the confinement effect on nanoconfined polymers. Recent studies reported a strong perturbation of local dynamics and substantial alteration of glass transition temperature Tg at nanoscale. However, how confinement affects the mechanical properties of polymers is not fully understood. Here, we show that the modulus of thin polymer films could be remarkedly altered through a polymer-polymer interface. The modulus of a thin polystyrene (PS) film next to a polydimethylsiloxane (PDMS) was determined from the PS-PDMS bilayer bulging test. A series of experiments show that the modulus of PS can be increased up to 37%, when the modulus of the neighboring PDMS varies from 1.04 to 4.88 MPa. The results demonstrate a strong sensitivity of mechanical properties of thin polymers to the hard/soft environment, which we attribute to the change of high-mobility layer by the polymer-polymer interface.

2.
Adv Mater ; : e2400158, 2024 Jun 07.
Artículo en Inglés | MEDLINE | ID: mdl-38847332

RESUMEN

Organic long-persistent luminescence (OLPL), which relies on energy storage for delayed light emission by the charge separation state, has attracted intense attention in various optical applications. However, charge separation (CS) is efficient only under ultraviolet excitation in most OLPL systems because it requires a driving force from the large energy difference between the local excited (LE) and charge transfer (CT) states. In this study, a multiresonance thermally activated delayed fluorescence (MR-TADF) molecule is incorporated into an exciplex system to achieve efficient OLPL in a composite material activated by visible light via a stepwise charge/energy transfer process. The enhanced absorption of the composite material facilitated a tenfold increase in the duration of the OLPL, which can last for several hours under visible light excitation. The excited state of the MR-TADF molecule tends to charge transfer to the acceptor, followed by energy transfer to the exciplex, which benefits from the small difference between the LE and CT states owing to the inherent CS characteristics of the opposing resonance effect. Afterglow displays of these composite materials are fabricated to demonstrate their considerable potential in encryption patterns and emergency lights, which take advantage of their excellent processability, visible light activation, and tunable luminescence properties.

3.
Nat Commun ; 15(1): 4856, 2024 Jun 07.
Artículo en Inglés | MEDLINE | ID: mdl-38849337

RESUMEN

Developing highly active materials that efficiently utilize solar spectra is crucial for photocatalysis, but still remains a challenge. Here, we report a new donor-acceptor (D-A) covalent organic framework (COF) with a wide absorption range from 200 nm to 900 nm (ultraviolet-visible-near infrared light). We find that the thiophene functional group is accurately introduced into the electron acceptor units of TpDPP-Py (TpDPP: 5,5'-(2,5-bis(2-ethylhexyl)-3,6-dioxo-2,3,5,6-tetrahydropyrrolo [3,4-c]pyrrole-1,4-diyl)bis(thiophene-2-carbaldehyde), Py: 1,3,6,8-tetrakis(4-aminophenyl)pyrene) COFs not only significantly extends its spectral absorption capacity but also endows them with two-photon and three-photon absorption effects, greatly enhancing the utilization rate of sunlight. The selective coupling of benzylamine as the target reactant is used to assess the photocatalytic activity of TpDPP-Py COFs, showing high photocatalytic conversion of 99% and selectivity of 98% in 20 min. Additionally, the TpDPP-Py COFs also exhibit the universality of photocatalytic selective coupling of other imine derivatives with ~100% conversion efficiency. Overall, this work brings a significant strategy for developing COFs with a wide absorption range to enhance photocatalytic activity.

4.
Appl Opt ; 63(14): D35-D40, 2024 May 10.
Artículo en Inglés | MEDLINE | ID: mdl-38856331

RESUMEN

Compact, magnetic field, B sensing is proposed and demonstrated by combining the two Faraday rotation elements and beam displacement crystals within a micro-optical fiber circulator with a fiber reflector and ferromagnets to allow high contrast attenuation in an optical fiber arm. Low optical noise sensing is measured at λ=1550n m as a change in attenuation, α, of optical light propagating through the rotators and back. The circulator's double-pass configuration, using a gold mirror as a reflector, achieves a magnetic field sensitivity s=Δ α/Δ B=(0.26±0.02)d B/m T with a resolution of Δ B=0.01m T, over a detection range B=0-89m T. The circulator as a platform provides direct connectivity to the Internet, allowing remote sensing to occur. The method described here is amenable to multisensor combinations, including with other sensor technologies, particularly in future integrated waveguide Faraday optical circuits and devices, extending its utility beyond point magnetic field sensing applications.

5.
J Hazard Mater ; 472: 134459, 2024 Jul 05.
Artículo en Inglés | MEDLINE | ID: mdl-38691999

RESUMEN

Bioaerosols are widely distributed in urban air and can be transmitted across the atmosphere, biosphere, and anthroposphere, resulting in infectious diseases. Automobile air conditioning (AAC) filters can trap airborne microbes. In this study, AAC filters were used to investigate the abundance and pathogenicity of airborne microorganisms in typical Chinese and European cities. Culturable bacteria and fungi concentrations were determined using microbial culturing. High-throughput sequencing was employed to analyze microbial community structures. The levels of culturable bioaerosols in Chinese and European cities exhibited disparities (Analysis of Variance, P < 0.01). The most dominant pathogenic bacteria and fungi were similar in Chinese (Mycobacterium: 18.2-18.9 %; Cladosporium: 23.0-30.2 %) and European cities (Mycobacterium: 15.4-37.7 %; Cladosporium: 18.1-29.3 %). Bartonella, Bordetella, Alternaria, and Aspergillus were also widely identified. BugBase analysis showed that microbiomes in China exhibited higher abundances of mobile genetic elements (MGEs) and biofilm formation capacity than those in Europe, indicating higher health risks. Through co-occurrence network analysis, heavy metals such as zinc were found to correlate with microorganism abundance; most bacteria were inversely associated, while fungi exhibited greater tolerance, indicating that heavy metals affect the growth and reproduction of bioaerosol microorganisms. This study elucidates the influence of social and environmental factors on shaping microbial community structures, offering practical insights for preventing and controlling regional bioaerosol pollution.


Asunto(s)
Aire Acondicionado , Microbiología del Aire , Automóviles , Bacterias , Ciudades , Hongos , China , Europa (Continente) , Bacterias/genética , Bacterias/aislamiento & purificación , Hongos/aislamiento & purificación , Hongos/patogenicidad , Hongos/genética , Filtros de Aire/microbiología , Contaminantes Atmosféricos/análisis , Microbiota , Monitoreo del Ambiente
6.
Food Sci Biotechnol ; 33(7): 1685-1696, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38623439

RESUMEN

American ginseng (Panax quinquefolium L.) is used as tonic plant and high-grade nourishment. Ultra-high-performance liquid chromatography-high resolution mass spectrometry (UHPLC-HRMS) method was established for identifying the chemical constituent in three morphological regions of American ginseng, including main root (MR), rhizome (RH) and lateral root (LR). The 63 saponins was identified in different morphological regions of 10 American ginseng samples. The chemical maker compounds in corresponding morphological region, while the major compounds of MR (malonyl-ginsenoside Rb1, ginsenoside Rd, Rs2 and pseudo-RC1), LR (stipuleanoside R2, ginsenoside Re and malonyl-ginsenoside Rc), and RH (malonyl-ginsenoside Rd, Rb3, and chikusetsu saponin II) were discovered. Correlation analysis showed that 11 compounds were positively correlated with the antioxidant activity of American ginseng. Supplementary Information: The online version contains supplementary material available at 10.1007/s10068-023-01453-4.

7.
Nat Commun ; 15(1): 3123, 2024 Apr 10.
Artículo en Inglés | MEDLINE | ID: mdl-38600179

RESUMEN

Stretchable neuromorphic optoelectronics present tantalizing opportunities for intelligent vision applications that necessitate high spatial resolution and multimodal interaction. Existing neuromorphic devices are either stretchable but not reconcilable with multifunctionality, or discrete but with low-end neurological function and limited flexibility. Herein, we propose a defect-tunable viscoelastic perovskite film that is assembled into strain-insensitive quasi-continuous microsphere morphologies for intrinsically stretchable neuromorphic vision-adaptive transistors. The resulting device achieves trichromatic photoadaptation and a rapid adaptive speed (<150 s) beyond human eyes (3 ~ 30 min) even under 100% mechanical strain. When acted as an artificial synapse, the device can operate at an ultra-low energy consumption (15 aJ) (far below the human brain of 1 ~ 10 fJ) with a high paired-pulse facilitation index of 270% (one of the best figures of merit in stretchable synaptic phototransistors). Furthermore, adaptive optical imaging is achieved by the strain-insensitive perovskite films, accelerating the implementation of next-generation neuromorphic vision systems.

8.
Adv Mater ; : e2400103, 2024 Apr 04.
Artículo en Inglés | MEDLINE | ID: mdl-38573809

RESUMEN

Hydrogel-based electronics have inherent similarities to biological tissues and hold potential for wearable applications. However, low conductivity, poor stretchability, nonpersonalizability, and uncontrollable dehydration during use limit their further development. In this study, projection stereolithography 3D printing high-conductive hydrogel for flexible passive wireless sensing is reported. The prepared photocurable silver-based hydrogel is rapidly planarized into antenna shapes on substrates using surface projection stereolithography. After partial dehydration, silver flakes within the circuits form sufficient conductive pathways to achieve high conductivity (387 S cm-1). By sealing the circuits to prevent further dehydration, the resistance remains stable when tensile strain is less than 100% for at least 30 days. Besides, the sealing materials provide versatile functionalities, such as stretchability and shape memory property. Customized flexible radio frequency identification tags are fabricated by integrating with commercial chips to complete the accurate recognition of eye movement, realizing passive wireless sensing.

9.
Angew Chem Int Ed Engl ; 63(19): e202319027, 2024 May 06.
Artículo en Inglés | MEDLINE | ID: mdl-38488819

RESUMEN

Heterocycle-linked phthalocyanine-based COFs with close-packed π-π conjugated structures are a kind of material with intrinsic electrical conductivity, and they are considered to be candidates for photoelectrical devices. Previous studies have revealed their applications for energy storage, gas sensors, and field-effect transistors. However, their potential application in photodetector is still not fully studied. The main difficulty is preparing high-quality films. In our study, we found that our newly designed benzimidazole-linked Cu (II)-phthalocyanine-based COFs (BICuPc-COFs) film can hardly formed with a regular aerobic oxidation method. Therefore, we developed a transfer dehydrogenation method with N-benzylideneaniline (BA) as a mild reagent. With this in hand, we successfully prepared a family of high crystalline BICuPc-COFs powders and films. Furthermore, both of these new BICuPc-COFs films showed high electrical conductivity (0.022-0.218 S/m), higher than most of the reported COFs materials. Due to the broad absorption and high conductivity of BICuPc-COFs, synaptic devices with small source-drain voltage (VDS=1 V) were fabricated with response light from visible to near-infrared. Based on these findings, we expect this study will provide a new perspective for the application of conducting heterocycle-linked COFs in synaptic devices.

10.
Nat Commun ; 15(1): 2624, 2024 Mar 23.
Artículo en Inglés | MEDLINE | ID: mdl-38521822

RESUMEN

Challenges associated with stretchable optoelectronic devices, such as pixel size, power consumption and stability, severely brock their realization in high-resolution digital imaging. Herein, we develop a universal detachable interface technique that allows uniform, damage-free and reproducible integration of micropatterned stretchable electrodes for pixel-dense intrinsically stretchable organic transistor arrays. Benefiting from the ideal heterocontact and short channel length (2 µm) in our transistors, switching current ratio exceeding 106, device density of 41,000 transistors/cm2, operational voltage down to 5 V and excellent stability are simultaneously achieved. The resultant stretchable transistor-based image sensors exhibit ultrasensitive X-ray detection and high-resolution imaging capability. A megapixel image is demonstrated, which is unprecedented for stretchable direct-conversion X-ray detectors. These results forge a bright future for the stretchable photonic integration toward next-generation visualization equipment.

11.
Nat Commun ; 15(1): 2397, 2024 Mar 16.
Artículo en Inglés | MEDLINE | ID: mdl-38493210

RESUMEN

Nanoclusters with atomically precise structures and discrete energy levels are considered as nanoscale semiconductors for artificial intelligence. However, nanocluster electronic engineering and optoelectronic behavior have remained obscure and unexplored. Hence, we create nanocluster photoreceptors inspired by mantis shrimp visual systems to satisfy the needs of compact but multi-task vision hardware and explore the photo-induced electronic transport. Wafer-scale arrayed photoreceptors are constructed by a nanocluster-conjugated molecule heterostructure. Nanoclusters perform as an in-sensor charge reservoir to tune the conductance levels of artificial photoreceptors by a light valve mechanism. A ligand-assisted charge transfer process takes place at nanocluster interface and it features an integration of spectral-dependent visual adaptation and circular polarization recognition. This approach is further employed for developing concisely structured, multi-task, and compact artificial visual systems and provides valuable guidelines for nanocluster neuromorphic devices.

12.
Natl Sci Rev ; 11(3): nwad253, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38312388

RESUMEN

Recent progress in multifunction-oriented high-mobility polymer semiconductors is profiled, with current challenges and future directions proposed in this perspective.

13.
J Chem Phys ; 160(4)2024 Jan 28.
Artículo en Inglés | MEDLINE | ID: mdl-38258926

RESUMEN

Optimizing mechanical performance is crucial for the practical utilization of stimuli-responsive polymers, while complex viscous and elastic behavior hinders a deep understanding of functional polymers under external field excitation. Here, we demonstrate the in situ dynamic and static mechanical responses under electric stimuli of poly(methyl methacrylate) (PMMA) above glass transition temperature (Tg) by applying a direct current electric field vertically to the mechanical loading. The results show that the electro-mechanical response of PMMA is directly correlated to chain relaxation modes with different length scales: for local segments, polarization provides resistance for molecular motion, manifested by enhanced moduli, increased transient viscosity, and a wider linear viscoelastic range, whereas in a larger spatial range, polarization-induced conformation change causes faster relaxation, reduced elastic modulus, and a lowered modulus plateau. Moreover, flow viscosity is reduced because of weaker friction between chain segments under polarization. Our results suggest effective strategies for precisely tuning the viscoelastic behavior of polymers above Tg through electric stimuli.

14.
Adv Mater ; 36(4): e2305987, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37639714

RESUMEN

Multifunctional semiconductors integrating unique optical, electrical, mechanical, and chemical characteristics are critical to advanced and emerging manufacturing technologies. However, due to the trade-off challenges in design principles, fabrication difficulty, defects in existing materials, etc., realizing multiple functions through multistage manufacturing is quite taxing. Here, an effective molecular design strategy is established to prepare a class of multifunctional integrated polymer semiconductors. The pyridal[1,2,3]triazole-thiophene co-structured tetrapolymers with full-backbone coplanarity and considerable inter/intramolecular noncovalent interactions facilitate short-range order and excellent (re)organization capability of polymer chains, providing stress-dissipation sites in the film state. The regioregular multicomponent conjugated backbones contribute to dense packing, excellent crystallinity, high crack onset strain over 100%, efficient carrier transport with mobilities exceeding 1 cm2  V-1  s-1 , and controllable near-infrared luminescence. Furthermore, a homologous blending strategy is proposed to further enhance the color-tunable luminescent properties of polymers while effectively retaining mechanical and electrical properties. The blended system exhibits excellent field-effect mobility (µ) and quantum yield (Φ), reaching a record Φ · µ of 0.43 cm2  V-1  s-1 . Overall, the proposed strategy facilitates a rational design of regioregular semicrystalline intrinsically stretchable polymers with high mobility and color-tunable intense luminescence, providing unique possibilities for the development of multifunctional integrated semiconductors in organic optoelectronics.

15.
Adv Mater ; 36(2): e2307326, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37849381

RESUMEN

Perovskites field-effect transistors (PeFETs) have been intensively investigated for their application in detector and synapse. However, synapse based on PeFETs is still very difficult to integrate excellent charge carrier transporting ability, photosensitivity, and nonvolatile memory effects into one device, which is very important for developing bionic electronic devices and edge computing. Here, two-dimensional (2D) perovskites are synthesized by incorporating fused π-conjugated pyrene-O-ethyl-ammonium (POE) ligands and a systematic study is conducted to obtain enhanced performance and reliable PeFETs. The optimized (POE)2 SnI4 transistors display the hole mobility over 0.3 cm2  V-1  s-1 , high repeatability, and operational stability. Meanwhile, the derived photo memory devices show remarkable photoresponse, with a switching ratio higher than 105 , high visible light responsivity (>4 × 104  A W-1 ), and stable storage-erase cycles, as well as competitive retention performance (104  s). The photoinduced memory behavior can be benefiting from the insulating nature of quantum-well in 2D perovskite under dark and its excellent light sensitivity. The excellent photo memory behaviors have been maintained after 40 days in a N2 atmosphere. Finally, a 2D perovskite-only transistors with a multi-level memory behavior (16 distinct states) is described by controlling incident light pulse. This work provides broader attention toward 2D perovskite and optoelectronic application.

16.
Adv Healthc Mater ; 13(10): e2303499, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38109414

RESUMEN

Chronic wound healing remains a substantial clinical challenge. Current treatments are often either prohibitively expensive or insufficient in meeting the various requirements needed for effective diabetic wound healing. A 4D printing multifunctional hydrogel dressing is reported here, which aligns perfectly with wounds owning various complex shapes and depths, promoting both wound closure and tissue regeneration. The hydrogel is prepared via digital light process (DLP) 3D printing of the mixture containing N-isopropylacrylamide (NIPAm), curcumin-loaded Pluronic F127 micelles (Cur-PF127), and poly(ethylene glycol) diacrylate-dopamine (PEGDA575-Do), a degradable crosslinker. The use of PEGDA575-Do ensures tissue adhesion and degradability, and cur-PF127 serves as an antibacterial agent. Moreover, the thermo-responsive mainchains (i.e., polymerized NIPAm) enables the activation of wound contraction by body temperature. The features of the prepared hydrogel, including robust tissue adhesion, temperature-responsive contraction, effective hemostasis, spectral antibacterial, biocompatibility, biodegradability, and inflammation regulation, contribute to accelerating diabetic wound healing in Methicillin-resistant Staphylococcus aureus (MRSA)-infected full-thickness skin defect diabetic rat models and liver injury mouse models, highlighting the potential of this customizable, mechanobiological, and inflammation-regulatory dressing to expedite wound healing in various clinical settings.


Asunto(s)
Diabetes Mellitus , Staphylococcus aureus Resistente a Meticilina , Ratones , Animales , Ratas , Hidrogeles/farmacología , Adherencias Tisulares , Cicatrización de Heridas , Antibacterianos/farmacología , Inflamación
17.
J Chem Phys ; 159(21)2023 Dec 07.
Artículo en Inglés | MEDLINE | ID: mdl-38054519

RESUMEN

The demand for applications, such as coatings, separation filters, and electronic packaging, has greatly driven the research of polymer films. At nanometer scale, mechanical properties of thin polymer films can significantly deviate from bulk. Despite outstanding progresses, there still lack deep discussions on nonlinear viscoelastic-viscoplastic response and their interactions under nanoconfinement. In this work, by conducting measurements via the bubble inflation method and modelling using Schapery and Perzyna equations, we demonstrate nonlinear viscoelastic-viscoplastic properties of freely standing thin polystyrene (PS) films. The results show the unchanged glassy compliance and the rubbery stiffening phenomenon for thin PS films, where the lower rubbery plateau in rubbery stiffening may originate from the induced molecular orientation by plastic deformation. With decreasing film thickness, viscosity and yield stress in viscoplasticity increase in an exponential and a linear trend, respectively, indicating the significant role of nanoconfinement effect on viscoplastic properties. These findings may reveal that there are many properties from linear viscoelasticity to nonlinear viscoelasticity-viscoplasticity that need to be explored and unveiled for sufficient understanding of the nanoconfinement effect on altering mechanical behavior of polymers.

18.
J Sep Sci ; 46(24): e2300473, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37933715

RESUMEN

Angelica sinensis (Oliv.) Diels. has been used for women to enrich the blood, prevent and treat blood deficiency syndrome in Traditional Chinese Medicine for thousands of years. Wine-processed Angelica sinensis, soil-processed Angelica sinensis, oil-processed Angelica sinensis, and charred-processed Angelica sinensis are the most significant four processed products used in Chinese clinic. However, there have been few studies aimed at comparing their chemical differences. Ultra-high-performance liquid chromatography coupled with quadrupole-orbitrap mass spectrometry combining with nontargeted metabolomics was applied to investigate the diversity of processed products of Angelica sinensis. A total of 74 compounds with the variable importance in the projection value more than 1.5 and P less than 0.05 in ANOVA were highlighted as the compounds that contribute most to the discrimination of Angelica sinensis and four processed products. The results showed the metabolic changes between Angelica sinensis and its four processed products, there were 19 metabolites, 3 metabolites, 6 metabolites, and 45 metabolites were tentatively assigned in soil-processed Angelica sinensis, wine-processed Angelica sinensis, oil-processed Angelica sinensis, and charred-processed Angelica sinensis, respectively. These results suggested that the proposed metabolomics approach was useful for the quality evaluation and control of processed products of Angelica sinensis.


Asunto(s)
Angelica sinensis , Medicamentos Herbarios Chinos , Humanos , Femenino , Medicamentos Herbarios Chinos/análisis , Angelica sinensis/química , Cromatografía Líquida de Alta Presión , Cromatografía de Gases y Espectrometría de Masas , Espectrometría de Masas , Metabolómica , Suelo
19.
Environ Sci Technol ; 57(41): 15580-15587, 2023 10 17.
Artículo en Inglés | MEDLINE | ID: mdl-37804225

RESUMEN

We present experimental evidence that atomic and molecular iodine, I and I2, are produced spontaneously in the dark at the air-water interface of iodide-containing droplets without any added catalysts, oxidants, or irradiation. Specifically, we observe I3- formation within droplets, and I2 emission into the gas phase from NaI-containing droplets over a range of droplet sizes. The formation of both products is enhanced in the presence of electron scavengers, either in the gas phase or in solution, and it clearly follows a Langmuir-Hinshelwood mechanism, suggesting an interfacial process. These observations are consistent with iodide oxidation at the interface, possibly initiated by the strong intrinsic electric field present there, followed by well-known solution-phase reactions of the iodine atom. This interfacial chemistry could be important in many contexts, including atmospheric aerosols.


Asunto(s)
Yodo , Agua , Agua/química , Yoduros/química , Yodo/química
20.
Sensors (Basel) ; 23(12)2023 Jun 06.
Artículo en Inglés | MEDLINE | ID: mdl-37420549

RESUMEN

Vehicle-mounted ground-penetrating radar (GPR) has been used to non-destructively inspect and evaluate railway subgrade conditions. However, existing GPR data processing and interpretation methods mostly rely on time-consuming manual interpretation, and limited studies have applied machine learning methods. GPR data are complex, high-dimensional, and redundant, in particular with non-negligible noises, for which traditional machine learning methods are not effective when applied to GPR data processing and interpretation. To solve this problem, deep learning is more suitable to process large amounts of training data, as well as to perform better data interpretation. In this study, we proposed a novel deep learning method to process GPR data, the CRNN network, which combines convolutional neural networks (CNN) and recurrent neural networks (RNN). The CNN processes raw GPR waveform data from signal channels, and the RNN processes features from multiple channels. The results show that the CRNN network achieves a higher precision at 83.4%, with a recall of 77.3%. Compared to the traditional machine learning method, the CRNN is 5.2 times faster and has a smaller size of 2.6 MB (traditional machine learning method: 104.0 MB). Our research output has demonstrated that the developed deep learning method improves the efficiency and accuracy of railway subgrade condition evaluation.


Asunto(s)
Aprendizaje Profundo , Radar , Redes Neurales de la Computación , Aprendizaje Automático
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