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1.
Biomaterials ; 312: 122744, 2025 Jan.
Article de Anglais | MEDLINE | ID: mdl-39106820

RÉSUMÉ

Inflammation within the central nervous system (CNS), which may be triggered by surgical trauma, has been implicated as a significant factor contributing to postoperative cognitive dysfunction (POCD). The relationship between mitigating inflammation at peripheral surgical sites and its potential to attenuate the CNS inflammatory response, thereby easing POCD symptoms, remains uncertain. Notably, carbon monoxide (CO), a gasotransmitter, exhibits pronounced anti-inflammatory effects. Herein, we have developed carbon monoxide-releasing micelles (CORMs), a nanoparticle that safely and locally liberates CO upon exposure to 650 nm light irradiation. In a POCD mouse model, treatment with CORMs activated by light (CORMs + hv) markedly reduced the concentrations of interleukin (IL)-6, IL-1ß, and tumor necrosis factor-alpha (TNF-α) in both the peripheral blood and the hippocampus, alongside a decrease in ionized calcium-binding adapter molecule 1 in the hippocampal CA1 region. Furthermore, CORMs + hv treatment diminished Evans blue extravasation, augmented the expression of tight junction proteins zonula occludens-1 and occludin, enhanced neurocognitive functions, and fostered fracture healing. Bioinformatics analysis and experimental validation has identified Htr1b and Trhr as potential key regulators in the neuroactive ligand-receptor interaction signaling pathway implicated in POCD. This work offers new perspectives on the mechanisms driving POCD and avenues for therapeutic intervention.


Sujet(s)
Monoxyde de carbone , Lumière , Complications post-opératoires cognitives , Animaux , Complications post-opératoires cognitives/étiologie , Complications post-opératoires cognitives/métabolisme , Mâle , Souris , Souris de lignée C57BL , Nanoparticules/composition chimique , Micelles ,
2.
Angew Chem Int Ed Engl ; : e202413827, 2024 Sep 07.
Article de Anglais | MEDLINE | ID: mdl-39243223

RÉSUMÉ

Smart materials enabling emission intensity or wavelength tuning by light stimulus attract attention in numerous cutting-edge fields. However, due to the generally dense molecular stacking against photoresponsivity in solid states, especially in crystals, developing rapidly phototunable solid-state luminescent systems remains challenging. Herein, we propose a new luminophore that serves as both a photoresponsive unit and a luminescent group, while possessing enhanced conformational freedom to provide a solution. Namely, photoexcitation-induced molecular conformational change of an ionized persulfurated arene based on weak intermolecular aliphatic C-H···π interaction was employed. On these basis, rapidly enhanced phosphorescence upon irradiation can be observed in a series of phase states, like solution state, crystal, and amorphous state, especially with a high photoresponsive rate of 0.033 s-1 in crystal state that is superior to the relevant reported cases. Moreover, a rapidly phototunable afterglow effect is achieved by extending this molecule into some polymer-based doping systems, endowing the system with unique dynamic imaging and fast photopatterning capabilities. Such a single-luminophore molecular engineering and the underlying mechanism have implications for building different condensed functional materials, principally for those with stimuli responses in solid states.

3.
Mikrochim Acta ; 191(10): 582, 2024 Sep 09.
Article de Anglais | MEDLINE | ID: mdl-39245663

RÉSUMÉ

A novel colorimetric approach specifically designed to effectively identify the presence of 3-aminophenol (3-AP) in environmental water is introduced. Briefly, a nitrogen-doped carbon-supported cobalt nanozyme (Co@CN-1) was synthesized and utilized to improve the oxidation of 3,3',5,5'-tetramethylbenzidine (TMB) in the presence of peroxymonosulfate (PMS). Comparative catalytic reactions confirmed that the performance of PMS as an activator exceeds that of hydrogen peroxide catalytically by a factor of 3.5. The catalytic reaction parameters underwent optimization, further resulting in the derivation of a linear detection equation for 3-AP, expressed as inhibition rate (IR%) = 3.35[3-AP]-4.36 (0-20 µM, R2 = 0.994) and IR% = 1.43[3-AP] + 31.87 (20-36 µM, R2 = 0.992), with the limit of detection (LOD) of 2.84 µM. The linear relationship between 3-AP concentration and the conversion of color to grayscale value (GSV) was established by smartphones, expressed as GSV = 1.28[3-AP] + 147.10 (R2 = 0.972). Density functional theory calculations revealed that Co acts as the preferred active site for donating electrons in PMS activation. This work provides a rapid and accurate approach for monitoring 3-AP concentration, enabling real-time analysis and potentially contributing to environmental and ecological studies.

4.
Phys Chem Chem Phys ; 26(25): 17809-17816, 2024 Jun 26.
Article de Anglais | MEDLINE | ID: mdl-38884121

RÉSUMÉ

Thermally activated delayed fluorescence (TADF) has been widely applied to electroluminescent materials to take the best advantage of triplet excitons. For some materials, the TADF originates from high-level reverse intersystem crossing (hRISC), and has attracted much attention due to its high efficiency for utilizing the triplet excitons. However, reports concerning the mechanistic studies on the hRISC-TADF process and structure-property correlation are sparse. In this study, we prepared three compounds containing triphenylamine and benzophenone with different substitution positions, o-TPA-BP, m-TPA-BP, and p-TPA-BP, in which only p-TPA-BP displays strong luminescence and hRISC-TADF features. To investigate the mechanism of the substituent-position-dependent hRISC-TADF, ultrafast time-resolved spectroscopy was utilized to observe the deactivation pathways with the assistance of theoretical calculations. The results show that o-TPA-BP will not generate triplet species, and the triplet species for m-TPA-BP will rapidly deactivate. Only p-TPA-BP can transition back to the singlet state from the T2 state effectively and exhibit a large gap between T1 and T2 to favor the hRISC route. These results illustrate how the substitution position affects the ISC and further influences the luminescence properties, which can provide new insights for developing new high-efficiency luminescent materials.

5.
Nat Commun ; 15(1): 4674, 2024 Jun 01.
Article de Anglais | MEDLINE | ID: mdl-38824140

RÉSUMÉ

Polymer-based pure organic room-temperature phosphorescent materials have tremendous advantages in applications owing to their low cost, vast resources, and easy processability. However, designing polymer-based room-temperature phosphorescent materials with large Stokes shifts as key requirements in biocompatibility and environmental-friendly performance is still challenging. By generating charge transfer states as the gangplank from singlet excited states to triplet states in doped organic molecules, we find a host molecule (pyrrolidone) that affords charge transfer with doped guest molecules, and excellent polymer-based organic room-temperature phosphorescent materials can be easily fabricated when polymerizing the host molecule. By adding polyaromatic hydrocarbon molecules as electron-donor in polyvinylpyrrolidone, efficient intersystem crossing and tunable phosphorescent from green to near-infrared can be achieved, with maximum phosphorescence wavelength and lifetime up to 757 nm and 3850 ms, respectively. These doped polyvinylpyrrolidone materials have good photoactivation properties, recyclability, advanced data encryption, and anti-counterfeiting. This reported design strategy paves the way for the design of polyvinylpyrrolidone-based room-temperature phosphorescent materials.

6.
Chem Sci ; 15(22): 8422-8429, 2024 Jun 05.
Article de Anglais | MEDLINE | ID: mdl-38846403

RÉSUMÉ

Designing artificial photocatalysts for CO2 reduction is challenging, mainly due to the intrinsic difficulty of making multiple functional units cooperate efficiently. Herein, three-dimensional metal covalent organic frameworks (3D MCOFs) were employed as an innovative platform to integrate a strong Ru(ii) light-harvesting unit, an active Re(i) catalytic center, and an efficient charge separation configuration for photocatalysis. The photosensitive moiety was precisely stabilized into the covalent skeleton by using a rational-designed Ru(ii) complex as one of the building units, while the Re(i) center was linked via a shared bridging ligand with an Ru(ii) center, opening an effective pathway for their electronic interaction. Remarkably, the as-synthesized MCOF exhibited impressive CO2 photoreduction activity with a CO generation rate as high as 1840 µmol g-1 h-1 and 97.7% selectivity. The femtosecond transient absorption spectroscopy combined with theoretical calculations uncovered the fast charge-transfer dynamics occurring between the photoactive and catalytic centers, providing a comprehensive understanding of the photocatalytic mechanism. This work offers in-depth insight into the design of MCOF-based photocatalysts for solar energy utilization.

7.
Chemistry ; 30(44): e202401084, 2024 Aug 06.
Article de Anglais | MEDLINE | ID: mdl-38819870

RÉSUMÉ

The link of an antenna dye with an electron spin converter, in this case naphthalenediimide and C60, produces a system with a rich photophysics including the detection of more than one triplet state on the long timescale (tens of µs). Beside the use of optical spectroscopies in the ns and in the fs time scale, we used time-resolved Electron Paramagnetic Resonance (TREPR) to study the system evolution following photoexcitation. TREPR keeps track of the formation path of the triplet states through specific spin polarization patterns observed in the spectra. The flexibility of the linker and solvent polarity play a role in favouring either electron transfer or energy transfer processes.

8.
Angew Chem Int Ed Engl ; 63(29): e202402774, 2024 Jul 15.
Article de Anglais | MEDLINE | ID: mdl-38584586

RÉSUMÉ

Currently, most photoredox catalysis polymerization systems are limited by high excitation power, long polymerization time, or the requirement of electron donors due to the precise design of efficient photocatalysts still poses a great challenge. Herein, we propose a new approach: the creation of efficient photocatalysts having low ground state oxidation potentials and high excited state energy levels, along with through-space charge transfer (TSCT) induced intersystem crossing (ISC) properties. A cabazole-naphthalimide (NI) dyad (NI-1) characterized by long triplet excited state lifetime (τT=62 µs), satisfactory ISC efficiency (ΦΔ=54.3 %) and powerful reduction capacity [Singlet: E1/2 (PC+1/*PC)=-1.93 eV, Triplet: E1/2 (PC+1/*PC)=-0.84 eV] was obtained. An efficient and rapid polymerization (83 % conversion of 1 mM monomer in 30 s) was observed under the conditions of without electron donor, low excitation power (10 mW cm-2) and low catalyst (NI-1) loading (<50 µM). In contrast, the conversion rate was lower at 29 % when the reference catalyst (NI-4) was used for photopolymerization under the same conditions, demonstrating the advantage of the TSCT photocatalyst. Finally, the TSCT material was used as a photocatalyst in practical lithography for the first time, achieving pattern resolutions of up to 10 µm.

9.
Radiology ; 311(1): e231461, 2024 04.
Article de Anglais | MEDLINE | ID: mdl-38652028

RÉSUMÉ

Background Noninvasive tests can be used to screen patients with chronic liver disease for advanced liver fibrosis; however, the use of single tests may not be adequate. Purpose To construct sequential clinical algorithms that include a US deep learning (DL) model and compare their ability to predict advanced liver fibrosis with that of other noninvasive tests. Materials and Methods This retrospective study included adult patients with a history of chronic liver disease or unexplained abnormal liver function test results who underwent B-mode US of the liver between January 2014 and September 2022 at three health care facilities. A US-based DL network (FIB-Net) was trained on US images to predict whether the shear-wave elastography (SWE) value was 8.7 kPa or higher, indicative of advanced fibrosis. In the internal and external test sets, a two-step algorithm (Two-step#1) using the Fibrosis-4 Index (FIB-4) followed by FIB-Net and a three-step algorithm (Three-step#1) using FIB-4 followed by FIB-Net and SWE were used to simulate screening scenarios where liver stiffness measurements were not or were available, respectively. Measures of diagnostic accuracy were calculated using liver biopsy as the reference standard and compared between FIB-4, SWE, FIB-Net, and European Association for the Study of the Liver guidelines (ie, FIB-4 followed by SWE), along with sequential algorithms. Results The training, validation, and test data sets included 3067 (median age, 42 years [IQR, 33-53 years]; 2083 male), 1599 (median age, 41 years [IQR, 33-51 years]; 1124 male), and 1228 (median age, 44 years [IQR, 33-55 years]; 741 male) patients, respectively. FIB-Net obtained a noninferior specificity with a margin of 5% (P < .001) compared with SWE (80% vs 82%). The Two-step#1 algorithm showed higher specificity and positive predictive value (PPV) than FIB-4 (specificity, 79% vs 57%; PPV, 44% vs 32%) while reducing unnecessary referrals by 42%. The Three-step#1 algorithm had higher specificity and PPV compared with European Association for the Study of the Liver guidelines (specificity, 94% vs 88%; PPV, 73% vs 64%) while reducing unnecessary referrals by 35%. Conclusion A sequential algorithm combining FIB-4 and a US DL model showed higher diagnostic accuracy and improved referral management for all-cause advanced liver fibrosis compared with FIB-4 or the DL model alone. © RSNA, 2024 Supplemental material is available for this article. See also the editorial by Ghosh in this issue.


Sujet(s)
Algorithmes , Imagerie d'élasticité tissulaire , Cirrhose du foie , Humains , Mâle , Cirrhose du foie/imagerie diagnostique , Adulte d'âge moyen , Femelle , Études rétrospectives , Imagerie d'élasticité tissulaire/méthodes , Adulte , Apprentissage profond , Foie/imagerie diagnostique , Foie/anatomopathologie , Sujet âgé , Échographie/méthodes
10.
Nat Commun ; 15(1): 2561, 2024 Mar 22.
Article de Anglais | MEDLINE | ID: mdl-38519517

RÉSUMÉ

Cocrystal engineering is an efficient and simple strategy to construct functional materials, especially for the exploitation of novel and multifunctional materials. Herein, we report two kinds of nucleic-acid-base cocrystal systems that imitate the strong hydrogen bond interactions constructed in the form of complementary base pairing. The two cocrystals studied exhibit different colors of phosphorescence from their monomeric counterparts and show the feature of rare high-temperature phosphorescence. Mechanistic studies reveal that the strong hydrogen bond network stabilizes the triplet state and suppresses non-radiative transitions, resulting in phosphorescence even at 425 K. Moreover, the isolation effects of the hydrogen bond network regulate the interactions between the phosphor groups, realizing the manipulation from aggregation to single-molecule phosphorescence. Benefiting from the long-lived triplet state with a high quantum yield, the generation of reactive oxygen species by energy transfer is also available to utilize for some applications such as in photodynamic therapy and broad-spectrum microbicidal effects. In vitro experiments show that the cocrystals efficiently kill bacteria on a tooth surface and significantly help prevent dental caries. This work not only provides deep insight into the relationship of the structure-properties of cocrystal systems, but also facilitates the design of multifunctional cocrystal materials and enriches their potential applications.


Sujet(s)
Anti-infectieux , Caries dentaires , Acides nucléiques , Humains , Cristallisation , Anti-infectieux/pharmacologie
11.
Int Immunopharmacol ; 131: 111858, 2024 Apr 20.
Article de Anglais | MEDLINE | ID: mdl-38492336

RÉSUMÉ

BACKGROUND: Diabetes is a global health problem whose common complication is diabetic cardiomyopathy, characterized by chronic inflammation of the heart muscle. Macrophages are the main white blood cells found in the resting heart. Therefore, we investigated the underling mechanism of macrophage on myocardial fibrosis in diabetes. METHODS: Here, echocardiography was utilized to evaluate cardiac function, and the degree of myocardial fibrosis was assessed using Masson's trichrome staining, followed by single-cell RNA sequencing (scRNA-seq) to analyze the phenotype, function, developmental trajectory, and interactions between immune cells, endothelial cells (ECs), and fibroblasts (FBs) in the hearts of db/db mice at different stages of diabetes. Macrophages and cardiac fibroblasts were also co-cultured in order to study the signaling between macrophages and fibroblasts. RESULTS: We found that with the development of diabetes mellitus, myocardial hypertrophy and fibrosis occurred that was accompanied by cardiac dysfunction. A significant proportion of immune cells, endothelial cells, and fibroblasts were identified by RNA sequencing. The most significant changes observed were in macrophages, which undergo M1 polarization and are critical for oxidative stress and extracellular matrix (ECM) formation. We further found that M1 macrophages secreted interleukin-1ß (IL-1ß), which interacted with the receptor on the surface of fibroblasts, to cause myocardial fibrosis. In addition, crosstalk between M1 macrophages and endothelial cells also plays a key role in fibrosis and immune response regulation through IL-1ß and corresponding receptors. CONCLUSIONS: M1 macrophages mediate diabetic myocardial fibrosis through interleukin-1ß interaction with fibroblasts.


Sujet(s)
Diabète , Cardiomyopathies diabétiques , Souris , Animaux , Interleukine-1 bêta , Cellules endothéliales , Macrophages , Fibrose
12.
Radiology ; 310(3): e232255, 2024 03.
Article de Anglais | MEDLINE | ID: mdl-38470237

RÉSUMÉ

Background Large language models (LLMs) hold substantial promise for medical imaging interpretation. However, there is a lack of studies on their feasibility in handling reasoning questions associated with medical diagnosis. Purpose To investigate the viability of leveraging three publicly available LLMs to enhance consistency and diagnostic accuracy in medical imaging based on standardized reporting, with pathology as the reference standard. Materials and Methods US images of thyroid nodules with pathologic results were retrospectively collected from a tertiary referral hospital between July 2022 and December 2022 and used to evaluate malignancy diagnoses generated by three LLMs-OpenAI's ChatGPT 3.5, ChatGPT 4.0, and Google's Bard. Inter- and intra-LLM agreement of diagnosis were evaluated. Then, diagnostic performance, including accuracy, sensitivity, specificity, and area under the receiver operating characteristic curve (AUC), was evaluated and compared for the LLMs and three interactive approaches: human reader combined with LLMs, image-to-text model combined with LLMs, and an end-to-end convolutional neural network model. Results A total of 1161 US images of thyroid nodules (498 benign, 663 malignant) from 725 patients (mean age, 42.2 years ± 14.1 [SD]; 516 women) were evaluated. ChatGPT 4.0 and Bard displayed substantial to almost perfect intra-LLM agreement (κ range, 0.65-0.86 [95% CI: 0.64, 0.86]), while ChatGPT 3.5 showed fair to substantial agreement (κ range, 0.36-0.68 [95% CI: 0.36, 0.68]). ChatGPT 4.0 had an accuracy of 78%-86% (95% CI: 76%, 88%) and sensitivity of 86%-95% (95% CI: 83%, 96%), compared with 74%-86% (95% CI: 71%, 88%) and 74%-91% (95% CI: 71%, 93%), respectively, for Bard. Moreover, with ChatGPT 4.0, the image-to-text-LLM strategy exhibited an AUC (0.83 [95% CI: 0.80, 0.85]) and accuracy (84% [95% CI: 82%, 86%]) comparable to those of the human-LLM interaction strategy with two senior readers and one junior reader and exceeding those of the human-LLM interaction strategy with one junior reader. Conclusion LLMs, particularly integrated with image-to-text approaches, show potential in enhancing diagnostic medical imaging. ChatGPT 4.0 was optimal for consistency and diagnostic accuracy when compared with Bard and ChatGPT 3.5. © RSNA, 2024 Supplemental material is available for this article.


Sujet(s)
Nodule thyroïdien , Humains , Femelle , Adulte , Nodule thyroïdien/imagerie diagnostique , Études rétrospectives , Langage , , Courbe ROC
13.
RSC Adv ; 14(7): 4503-4508, 2024 Jan 31.
Article de Anglais | MEDLINE | ID: mdl-38312733

RÉSUMÉ

Organic cocrystal engineering provides a promising route to promote the near-infrared (NIR) light harvesting and photothermal conversion (PTC) abilities of small organic molecules through the rich noncovalent bond interactions of D/A units. Besides, the single-bond rotatable groups known as "rotors" are considered to be conducive to the nonradiative transitions of the excited states of organic molecules. Herein, we propose a single-/double-bond dual-rotor strategy to construct D-A cocrystals for NIR PTC application. The results reveal that the cocrystal exhibits an ultra-broadband absorption from 300 nm to 2000 nm profiting from the strong π-π stacking and charge transfer interactions, and the weakened p-π interaction. More importantly, the PTC efficiency of cocrystals at 1064 nm in the NIR-II region can be largely enhanced by modulating the number of rotor groups and the F-substituents of D/A units. As is revealed by fs-TA spectroscopy, the superior NIR PTC performance can be attributed to the nonradiative decays of excited states induced by the free rotation of the single-bond rotor (-CH3) from the donors and the inactive double-bond rotor ([double bond, length as m-dash]C(C[triple bond, length as m-dash]N)2) being in the active form of [-C(C[triple bond, length as m-dash]N)2] in the excited states from the acceptors. This prototype displays a promising route to extend the functionalization of small organic molecules based on organic cocrystal engineering.

14.
Chem Commun (Camb) ; 60(17): 2385-2388, 2024 Feb 22.
Article de Anglais | MEDLINE | ID: mdl-38321968

RÉSUMÉ

We present a red light-activated zincII bis(dipyrrin) symmetry breaking charge transfer (SBCT) architecture, showing a large molar absorption coefficient (ε = 15.4 × 104 M-1 cm-1), high reactive singlet oxygen generation efficiency (ΦΔ ≈ 0.8) and long-lived triplet state (τT = 150 µs) compared to the donor-acceptor analogue dipyrrin-BF2 complex, highlighting the superiority of the SBCT approach. For the first time, we demonstrated the potential of a SBCT scaffold in red-light-induced methyl methacrylate (MMA) polymerization, using a dual photocatalyst excitation approach.

15.
Langmuir ; 40(8): 4410-4423, 2024 Feb 27.
Article de Anglais | MEDLINE | ID: mdl-38348971

RÉSUMÉ

In this paper, we report results on the electronic structure and transport properties of molecular junctions fabricated via conducting probe atomic force microscopy (CP-AFM) using self-assembled monolayers (SAMs) of n-alkyl chains anchored with acetylene groups (CnA; n = 8, 9, 10, and 12) on Ag, Au, and Pt electrodes. We found that the current-voltage (I-V) characteristics of CnA CP-AFM junctions can be very accurately reproduced by the same off-resonant single-level model (orSLM) successfully utilized previously for many other junctions. We demonstrate that important insight into the energy-level alignment can be gained from experimental data of transport (processed via the orSLM) and ultraviolet photoelectron spectroscopy combined with ab initio quantum chemical information based on the many-body outer valence Green's function method. Measured conductance GAg < GAu < GPt is found to follow the same ordering as the metal work function ΦAu < ΦAu < ΦPt, a fact that points toward a transport mediated by an occupied molecular orbital (MO). Still, careful data analysis surprisingly revealed that transport is not dominated by the ubiquitous HOMO but rather by the HOMO-1. This is an important difference from other molecular tunnel junctions with p-type HOMO-mediated conduction investigated in the past, including the alkyl thiols (CnT) to which we refer in view of some similarities. Furthermore, unlike in CnT and other junctions anchored with thiol groups investigated in the past, the AFM tip causes in CnA an additional MO shift, whose independence of size (n) rules out significant image charge effects. Along with the prevalence of the HOMO-1 over the HOMO, the impact of the "second" (tip) electrode on the energy level alignment is another important finding that makes the CnA and CnT junctions different. What ultimately makes CnA unique at the microscopic level is a salient difference never reported previously, namely, that CnA's alkyne functional group gives rise to two energetically close (HOMO and HOMO-1) orbitals. This distinguishes the present CnA from the CnT, whose HOMO stemming from its thiol group is well separated energetically from the other MOs.

16.
J Phys Chem Lett ; 15(4): 959-968, 2024 Feb 01.
Article de Anglais | MEDLINE | ID: mdl-38252167

RÉSUMÉ

To study the intersystem crossing (ISC) and the spatial confinement of the triplet excited states of organic chromophores, we prepared a series of Bodipy dimers. We found that the connection position of the two units has a significant effect on the absorption and fluorescence. Singlet oxygen quantum yields of 3.8-12.4% were observed for the dimers, which are independent of solvent polarity. Nanosecond transient absorption spectra indicate the population of long-lived triplet excited states with lifetimes (τT) of 45-454 µs. Pulsed laser-excited time-resolved electron paramagnetic resonance (TREPR) spectra show that the T1 triplet states are essentially delocalized, which is different from the case for the previously reported Bodipy dimers. The TREPR spectra of the triplet states imply that the delocalization over the whole dimer essentially depends on the electron density of the carbon atoms at the connection sites. This property may become a universal rule for controlling the T1 state confinement in multichromophore organic molecules.

17.
Angew Chem Int Ed Engl ; 63(10): e202318628, 2024 Mar 04.
Article de Anglais | MEDLINE | ID: mdl-38225206

RÉSUMÉ

An anion-counterion strategy is proposed to construct organic mono-radical charge-transfer cocrystals for near-infrared photothermal conversion and solar-driven water evaporation. Ionic compounds with halogen anions as the counterions serve as electron donors, providing the necessary electrons for efficient charge transfer with unchanged skeleton atoms and structures as well as the broad red-shifted absorption (200-2000 nm) and unprecedented photothermal conversion efficiency (~90.5 %@808 nm) for the cocrystals. Based on these cocrystals, an excellent solar-driven interfacial water evaporation rate up to 6.1±1.1 kg ⋅ m-2 ⋅ h-1 under 1 sun is recorded due to the comprehensive evaporation effect from the cocrystal loading in polyurethane foams and chimney addition, such performance is superior to the reported results on charge-transfer cocrystals or other materials for solar-driven interfacial evaporation. This prototype exhibits the great potential of cocrystals prepared by the one-step mechanochemistry method in practical large-scale seawater desalination applications.

18.
J Phys Chem Lett ; 15(1): 68-75, 2024 Jan 11.
Article de Anglais | MEDLINE | ID: mdl-38131660

RÉSUMÉ

The specific stacking mode of D/A blocks is often considered to largely determine the physicochemical properties of cocrystals. However, this rule may fail when encountering a large degree of (integer or near-integer) charge transfer situations. Herein, we explore the extensive correlations between the possible smallest structural units, stacking modes, and near-infrared photothermal conversion (NIR-PTC) properties of F4TCNQ-based cocrystals with typical features of integer-charge-transfer. Surprisingly, these cocrystals with distinct stacking modes display analogous D-A interactions, broad red-shift absorption, ultrafast (1-3 ps) relaxation dynamics of excited states, and excellent NIR-PTC properties. This supports that the resulting "D+A-" ion pairs from integer-charge-transfer may serve as the primary structural units beneath the secondary stacking modes to dominate the property of cocrystals. The stacking modes play an important but only secondary role. This work provides new insights into the structure-dynamics-property correlations and modular design of organic cocrystals for PTC and other applications.

19.
Genomics ; 116(1): 110767, 2024 01.
Article de Anglais | MEDLINE | ID: mdl-38128705

RÉSUMÉ

OBJECTIVE: Primary Sjögren's syndrome (pSS) is a intricate autoimmune disease mainly characterized of immune-mediated destruction of exocrine tissues, such as salivary and lacrimal glands, occurring dry mouth and eyes. Although some breakthroughs in understanding pSS have been uncovered, many questions remain about its pathogenesis, especially the internal relations between exocrine glands and secretions. METHOD: Transcriptomic and proteomic analyses were conducted on salivary tissues and saliva in experimental Sjögren syndrome (ESS). The ESS model was established by immunization with salivary gland protein. The expression of mRNAs and proteins in salivary tissues and saliva were determined by high-throughput sequencing transcriptomic analysis and LC-MS/MS-based proteome, respectively. Gene Ontology (GO) and Kyoto Encyclopedia of Genes and Genomes (KEGG) pathway analysis were used to recognize dysregulated genes and proteins. The association between RNA and protein abundance was investigated to provides a comprehensive understanding of RNA-protein correlations in the pathogenesis of pSS. RESULTS: As a result, we successfully established the ESS model. We recognized 3221 differentially expressed genes (DEGs) and 253 differentially expressed proteins (DEPs). The sample analysis showed that 61 proteins overlapped through the integrative analysis of transcriptomics and proteomics data. The enrichment pathway analysis of DEGs and DEPs in samples showed alterations in renin-angiotensin-system (RAS), lysosome, and apoptosis. Notably, we found that some genes, such as AGT, FN1, Klk1b26, Klk1, Klk1b5, Klk1b3 had a consistent trend in the regulation at the RNA and protein levels and might be potential diagnostic biomarkers of pSS. CONCLUSION: Herein, we found critical processes and potential biomakers that may contribute to pSS pathogenesis by analyzing dysregulated genes and pathways. Additionally, the integrative multi-omics datasets provided additional insight into understanding complicated disease mechanisms.


Sujet(s)
Syndrome de Gougerot-Sjögren , Humains , Syndrome de Gougerot-Sjögren/génétique , Syndrome de Gougerot-Sjögren/diagnostic , Syndrome de Gougerot-Sjögren/métabolisme , Transcriptome , Protéome/génétique , Chromatographie en phase liquide , Protéomique , Spectrométrie de masse en tandem , ARN
20.
Article de Anglais | MEDLINE | ID: mdl-38083514

RÉSUMÉ

Contrast-enhanced ultrasound (CEUS) video plays an important role in post-ablation treatment response assessment in patients with hepatocellular carcinoma (HCC). However, the assessment of treatment response using CEUS video is challenging due to issues such as high inter-frame data repeatability, small ablation area and poor imaging quality of CEUS video. To address these issues, we propose a two-stage diagnostic framework for post-ablation treatment response assessment in patients with HCC using CEUS video. The first stage is a location stage, which is used to locate the ablation area. At this stage, we propose a Yolov5-SFT to improve the location results of the ablation area and a similarity comparison module (SCM) to reduce data repeatability. The second stage is an assessment stage, which is used for the evaluation of postoperative efficacy. At this stage, we design an EfficientNet-SK to improve assessment accuracy. The Experimental results on the self-collected data show that the proposed framework outperforms other selected algorithms, and can effectively assist doctors in the assessment of post-ablation treatment response.


Sujet(s)
Carcinome hépatocellulaire , Tumeurs du foie , Humains , Carcinome hépatocellulaire/imagerie diagnostique , Carcinome hépatocellulaire/chirurgie , Tumeurs du foie/imagerie diagnostique , Tumeurs du foie/chirurgie , Produits de contraste , Tomodensitométrie , Échographie/méthodes
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