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1.
Opt Express ; 32(6): 9161-9170, 2024 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-38571155

RESUMO

Reflective cholesteric liquid crystal (CLC) Pancharatnam-Berry phase lens (PBL) devices have attracted significant attention in augmented reality (AR) display due to their wide spectral and angular response bandwidths, high diffraction efficiency, and polarization selectivity. However, currently reported CLC reflective PBLs are either limited by monochrome display or suffers from complicated design for colorful display. Herein, we demonstrate a colorful multi-plane AR display system with dynamically tunable reflective PBL. The reflective PBL is fabricated by polymer-stabilized cholesteric liquid crystal (PSCLC) that provides dynamical and continuous tunability of color and focal length by direct current (DC) voltage. A proof-of-concept colorful multi-plane AR device is demonstrated, where over 90% diffraction efficiency at desired wavelength has been obtained. The proposed simple, compact, and light AR display system capable of color-imaging with multi-depth shows great application potential in the vehicle-mounted head-up display (HUD).

2.
J Med Internet Res ; 26: e58013, 2024 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-39008845

RESUMO

BACKGROUND: Nonadherence to medication among patients with cardiovascular diseases undermines the desired therapeutic outcomes. eHealth interventions emerge as promising strategies to effectively tackle this issue. OBJECTIVE: The aim of this study was to conduct a network meta-analysis (NMA) to compare and rank the efficacy of various eHealth interventions in improving medication adherence among patients with cardiovascular diseases (CVDs). METHODS: A systematic search strategy was conducted in PubMed, Embase, Web of Science, Cochrane, China National Knowledge Infrastructure Library (CNKI), China Science and Technology Journal Database (Weipu), and WanFang databases to search for randomized controlled trials (RCTs) published from their inception on January 15, 2024. We carried out a frequentist NMA to compare the efficacy of various eHealth interventions. The quality of the literature was assessed using the risk of bias tool from the Cochrane Handbook (version 2.0), and extracted data were analyzed using Stata16.0 (StataCorp LLC) and RevMan5.4 software (Cochrane Collaboration). The certainty of evidence was evaluated using the Grading of Recommendations, Assessment, Development, and Evaluations (GRADE) approach. RESULTS: A total of 21 RCTs involving 3904 patients were enrolled. The NMA revealed that combined interventions (standardized mean difference [SMD] 0.89, 95% CI 0.22-1.57), telephone support (SMD 0.68, 95% CI 0.02-1.33), telemonitoring interventions (SMD 0.70, 95% CI 0.02-1.39), and mobile phone app interventions (SMD 0.65, 95% CI 0.01-1.30) were statistically superior to usual care. However, SMS compared to usual care showed no statistical difference. Notably, the combined intervention, with a surface under the cumulative ranking curve of 79.3%, appeared to be the most effective option for patients with CVDs. Regarding systolic blood pressure and diastolic blood pressure outcomes, the combined intervention also had the highest probability of being the best intervention. CONCLUSIONS: The research indicates that the combined intervention (SMS text messaging and telephone support) has the greatest likelihood of being the most effective eHealth intervention to improve medication adherence in patients with CVDs, followed by telemonitoring, telephone support, and app interventions. The results of these network meta-analyses can provide crucial evidence-based support for health care providers to enhance patients' medication adherence. Given the differences in the design and implementation of eHealth interventions, further large-scale, well-designed multicenter trials are needed. TRIAL REGISTRATION: INPLASY 2023120063; https://inplasy.com/inplasy-2023-12-0063/.


Assuntos
Doenças Cardiovasculares , Adesão à Medicação , Telemedicina , Humanos , Doenças Cardiovasculares/tratamento farmacológico , Adesão à Medicação/estatística & dados numéricos , Ensaios Clínicos Controlados Aleatórios como Assunto
3.
J Environ Manage ; 360: 121196, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38763117

RESUMO

At present, biochar has a large application potential in soil amelioration, pollution remediation, carbon sequestration and emission reduction, and research on the effect of biochar on soil ecology and environment has made positive progress. However, under natural and anthropogenic perturbations, biochar may undergo a series of environmental behaviors such as migratory transformation, mineralization and decomposition, and synergistic transport, thus posing certain potential risks. This paper outlines the multi-interfacial migration pathway of biochar in "air-soil-plant-animal-water", and analyzes the migration process and mechanism at different interfaces during the preparation, transportation and application of biochar. The two stages of the biochar mineralization process (mineralization of easily degradable aliphatic carbon components in the early stage and mineralization of relatively stable aromatic carbon components in the later stage) were described, the self-influencing factors and external environmental factors of biochar mineralization were analyzed, and the mineral stabilization mechanism and positive/negative excitation effects of biochar into the soil were elucidated. The proximity between field natural and artificially simulated aging of biochar were analyzed, and the change of its properties showed a trend of biological aging > chemical aging > physical aging > natural aging, and in order to improve the simulation and prediction, the artificially simulated aging party needs to be changed from a qualitative method to a quantitative method. The technical advantages, application scope and potential drawbacks of different biochar modification methods were compared, and biological modification can create new materials with enhanced environmental application. The stability performance of modified biochar was compared, indicating that raw materials, pyrolysis temperature and modification method were the key factors affecting the stability of biochar. The potential risks to the soil environment from different pollutants carried by biochar were summarized, the levels of pollutants released from biochar in the soil environment were highlighted, and a comprehensive selection of ecological risk assessment methods was suggested in terms of evaluation requirements, data acquisition and operation difficulty. Dynamic tracing of migration decomposition behavior, long-term assessment of pollution remediation effects, and directional design of modified composite biochar materials were proposed as scientific issues worthy of focused attention. The results can provide a certain reference basis for the theoretical research and technological development of biochar.


Assuntos
Carvão Vegetal , Ecossistema , Solo , Carvão Vegetal/química , Solo/química , Medição de Risco , Poluentes do Solo , Ecologia
4.
J Biomed Inform ; 146: 104485, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37660960

RESUMO

OBJECTIVE: We propose FedScore, a privacy-preserving federated learning framework for scoring system generation across multiple sites to facilitate cross-institutional collaborations. MATERIALS AND METHODS: The FedScore framework includes five modules: federated variable ranking, federated variable transformation, federated score derivation, federated model selection and federated model evaluation. To illustrate usage and assess FedScore's performance, we built a hypothetical global scoring system for mortality prediction within 30 days after a visit to an emergency department using 10 simulated sites divided from a tertiary hospital in Singapore. We employed a pre-existing score generator to construct 10 local scoring systems independently at each site and we also developed a scoring system using centralized data for comparison. RESULTS: We compared the acquired FedScore model's performance with that of other scoring models using the receiver operating characteristic (ROC) analysis. The FedScore model achieved an average area under the curve (AUC) value of 0.763 across all sites, with a standard deviation (SD) of 0.020. We also calculated the average AUC values and SDs for each local model, and the FedScore model showed promising accuracy and stability with a high average AUC value which was closest to the one of the pooled model and SD which was lower than that of most local models. CONCLUSION: This study demonstrates that FedScore is a privacy-preserving scoring system generator with potentially good generalizability.

5.
Appl Opt ; 62(1): 133-141, 2023 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-36606858

RESUMO

An end-to-end deep learning model based on the deep belief network (DBN) and gated recurrent unit (GRU) is proposed to recognize the single disturbance events and composite disturbance events in the phase-sensitive optical time-domain reflectometer (φ-OTDR). Making use of the DBN to fit the original data, five kinds of single disturbance events can be effectively recognized with the GRU network as the classifier. An average recognition accuracy of 96.72% with a short recognition time of 0.079 s can be achieved for single disturbance events. Moreover, the proposed method is also applied for recognizing composite disturbance events. Four kinds of composite disturbance events can be recognized with an average recognition accuracy as high as 90.94%, and the corresponding recognition time is only 0.084 s. Up until now, there have been fewer reports about the recognition of composite disturbance events in φ-OTDR systems. High recognition accuracy and short recognition time make the model based on DBN-GRU more capable in a high sensitivity, real-time φ-OTDR system.

6.
Health Commun ; 37(13): 1650-1660, 2022 11.
Artigo em Inglês | MEDLINE | ID: mdl-33866871

RESUMO

Individuals with social anxiety disorder (iSAD) experience adverse outcomes in daily life due to the disorder (e.g., lower educational and work achievement compared to their healthy counterparts). They are prone to social isolation, even though they desire intimate interpersonal relationships. Yet, little research on iSAD is devoted to understanding in detail a) when they interpret social situations as social-anxiety-provoking, b) how this interpretation motivates their assessments of their efficacy and likely interaction outcomes, and c) how they choose specific information-seeking strategies in uncertain social situations. Leveraging the theory of motivated information management (TMIM) and the emotional systems (ES) model, we explored the lived experiences of iSAD. We conducted in-depth interviews (N = 27) and analyzed them using thematic analysis. iSAD perceived discrepancies in a) mutual goals, b) common ground, and c) self-image as social-anxiety-provoking. These interpretations motivated their assessments of a) socializing benefits, b) communication competency, and c) interactant partner's amiability, which led to a mix of information-seeking decisions in social situations. Practical and theoretical implications for future research are discussed.


Assuntos
Fobia Social , Ansiedade , Humanos , Relações Interpessoais , Solidão , Fobia Social/terapia , Estudantes/psicologia , Incerteza
7.
Phytother Res ; 36(11): 4167-4182, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35778992

RESUMO

Hepatocytes has been confirmed to undergo EMT and can be converted into myofibroblasts during hepatic fibrogenesis. However, the mechanism of hepatocyte EMT regulation in hepatic fibrosis, particularly through HSP27 (human homologue of rodent HSP25), remains unclear. Mangiferin (MAN), a compound extracted from Mangifera indica L, has been reported to attenuate liver injury. This study aimed to investigate the mechanisms underlying HSP27 inhibition and the anti-fibrotic effect of MAN in liver fibrosis. Our results revealed that the expression of HSP27 was remarkably increased in the liver tissues of patients with liver cirrhosis and CCl4 -induced fibrotic rats. However, HSP27 shRNA treatment significantly alleviated fibrosis. Furthermore, MAN was found to inhibit CCl4 - and TGF-ß1-induced liver fibrosis and reduced hepatocyte EMT. More importantly, MAN decreased HSP27 expression to suppress the JAK2/STAT3 pathway, and subsequently blocked TGF-ß1/Smad signaling, which were consistent with its protection against CCl4 -induced EMT and liver fibrosis. Together, these results suggest that HSP27 may play a crucial role in hepatocyte EMT and liver fibrosis by activating JAK2/STAT3 signaling and TGF-ß1/Smad pathway. The suppression of HSP27 expression by MAN may be a novel strategy for attenuating the hepatocyte EMT in liver fibrosis.


Assuntos
Transição Epitelial-Mesenquimal , Fator de Crescimento Transformador beta1 , Animais , Humanos , Ratos , Fibrose , Hepatócitos , Proteínas de Choque Térmico HSP27/metabolismo , Janus Quinase 2 , Cirrose Hepática/tratamento farmacológico , Fator de Transcrição STAT3/metabolismo , Fator de Crescimento Transformador beta1/metabolismo , Proteínas Smad/metabolismo
8.
Org Biomol Chem ; 13(31): 8379-92, 2015 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-26086203

RESUMO

The discovery of a series of novel organic reactions has made methylenecyclopropanes (MCPs) some of the most popular building blocks in synthetic organic chemistry during the past two decades. Among reported works, the construction of heterocycles from MCPs has highlighted new synthetic methodologies that afford more opportunities for the quick synthesis of elaborately substituted products, and this should draw a great deal of attention. However, reviews in this area are insufficient, and the latest monograph on heterocycle synthesis from MCPs was published 12 years ago. This review aims to summarize the novel organic reactions of MCPs to produce heterocycles published in recent years, which have provided specific and powerful tools for organic synthesis.


Assuntos
Técnicas de Química Sintética/métodos , Ciclopropanos/química , Compostos Heterocíclicos/química , Compostos Heterocíclicos/síntese química
9.
Acta Crystallogr Sect E Struct Rep Online ; 70(Pt 6): o721, 2014 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-24940290

RESUMO

In the title compound, C16H10N4O2·0.17H2O, prepared by the one-step condensation reaction of isatin with hydrazine hydrate under microwave irradiation, the complete organic mol-ecule is generated by crystallographic inversion symmetry and therefore exists in an S-trans conformation. In the crystal, mol-ecules are linked by N-H⋯O hydrogen bonds, generating a three-dimensional framework with [001] channels, which are occupied by the disordered water mol-ecules.

10.
Foods ; 13(7)2024 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-38611433

RESUMO

Although the triglyceride form is the natural form of fish oil found in fish, the ethyl ester form of fish oil, which is used during processing to save costs, is also present on the market. In this study, fatty acids and lipids were determined using gas chromatography-mass spectrometry (GC-MS) and liquid chromatography-linear ion trap mass spectrometry (LC-LIT/MS), respectively, according to developed methods. The identification of fatty acids was based on the mass spectral characteristics and equivalent chain lengths. However, the fatty acid contents of both forms of fish oils are quite similar. The application of the LC-LIT/MS method for the structural characterization of triacylglycerols (TAGs) and the mechanism of LIT/MS fragmentation are also discussed. Neutral losses of CH2=CH2 (m/z 28) and CH3CH2OH (m/z 46), which are LIT/MS characteristics of ethyl ester from fish oil, were found for the first time. The triglyceride form of fish oils was easily and accurately identified using fingerprint chromatography. In conclusion, lipid analysis combined with LC-LIT/MS showed an improved capability to distinguish between types of fish oil.

11.
Sci Total Environ ; 921: 170928, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38367716

RESUMO

The fate of dissolved organic matter (DOM) is primarily governed by its sources, degradation, and transformation processes within the environment. However, the influence of metal-DOM complexation on DOM degradation remains ambiguous. In this study, controlled laboratory experiments were conducted using Cu(II) and natural water from the Duliujian River and the Beidagang Wetland to examine the effects of metal-DOM binding on the degradation pathway of DOM. Our results showed that Cu(II)-DOM complexation affected the distribution of DOM molecular weight with elevated Mw after complexed with Cu(II). Nevertheless, the concentration of DOM decreased over the incubation period due to degradation. In the absence of Cu(II) binding, both wetland and river DOM followed similar degradation pathways, transforming from high to low molecular weight with changes predominantly in the 1-10 kDa size-fraction during DOM degradation. In contrast, in the presence of Cu(II) and thus Cu(II)-DOM binding, the degradation of DOM was enhanced, resulting in higher kinetic rate constants for both wetland and river DOM. The results of differential spectra further confirmed the degradation of DOM with a decrease in bulk spectroscopic properties and an increase in the degree of DOM-Cu(II) complexation. These findings imply a mutually reinforcing relationship between metal-DOM complexation and the degradation of DOM in aquatic environments, providing new insights into the biogeochemical behavior and environmental fate of DOM.

12.
Int J Biol Macromol ; 275(Pt 2): 133333, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38945724

RESUMO

Fat and its hydrolysis products, fatty acids, are indispensable nutritional components; however, prolonged excessive fat consumption, particularly in western diets, contributes to the onset of obesity and multiple metabolic disorders. In this study, we propose a daily-ingestible hydrogel (denoted as ßC-MA hydrogel) composed of natural ß-glucan and sodium carboxymethylcellulose crosslinked by malic acid at 120 °C. This hydrogel exhibits rapid swelling performance, up to 24-fold within 1 min and 176-fold after 1 h in deionized water. It also lengthens gastric retention and increases endogenous satiety signal levels, potentially controlling appetite and reducing food intake. Furthermore, ßC-MA hydrogels that enter the small intestine can effectively inhibit fat hydrolysis and decrease triglyceride synthesis and transport. Specifically, the hydrogels inhibit the release of free fatty acids (FFAs) by approximately 50 % during digestion, influence the translocation of triglycerides and FFAs across the intestinal epithelium, and reduce the serum triglyceride levels by 22.2 %. These findings suggest that ßC-MA hydrogels could serve as a noninvasive gastrointestinal device for weight control, with the advantage of reducing food intake and restoring lipid metabolism homeostasis.


Assuntos
Hidrogéis , beta-Glucanas , Hidrogéis/química , beta-Glucanas/química , beta-Glucanas/farmacologia , Hidrólise , Animais , Triglicerídeos/metabolismo , Masculino , Camundongos , Metabolismo dos Lipídeos/efeitos dos fármacos , Ácidos Graxos não Esterificados/metabolismo , Trato Gastrointestinal/metabolismo , Trato Gastrointestinal/efeitos dos fármacos , Resposta de Saciedade/efeitos dos fármacos , Ratos
13.
Nurse Educ ; 2024 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-38981035

RESUMO

BACKGROUND: The performance of GPT-4 in nursing examinations within the Chinese context has not yet been thoroughly evaluated. OBJECTIVE: To assess the performance of GPT-4 on multiple-choice and open-ended questions derived from nursing examinations in the Chinese context. METHODS: The data sets of the Chinese National Nursing Licensure Examination spanning 2021 to 2023 were used to evaluate the accuracy of GPT-4 in multiple-choice questions. The performance of GPT-4 on open-ended questions was examined using 18 case-based questions. RESULTS: For multiple-choice questions, GPT-4 achieved an accuracy of 71.0% (511/720). For open-ended questions, the responses were evaluated for cosine similarity, logical consistency, and information quality, all of which were found to be at a moderate level. CONCLUSION: GPT-4 performed well at addressing queries on basic knowledge. However, it has notable limitations in answering open-ended questions. Nursing educators should weigh the benefits and challenges of GPT-4 for integration into nursing education.

14.
NPJ Digit Med ; 7(1): 209, 2024 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-39127820

RESUMO

Artificial intelligence (AI) has been extensively researched in medicine, but its practical application remains limited. Meanwhile, there are various disparities in existing AI-enabled clinical studies, which pose a challenge to global health equity. In this study, we conducted an in-depth analysis of the geo-economic distribution of 159 AI-enabled clinical studies, as well as the gender disparities among these studies. We aim to reveal these disparities from a global literature perspective, thus highlighting the need for equitable access to medical AI technologies.

15.
ACS Appl Mater Interfaces ; 16(26): 33021-33037, 2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38888460

RESUMO

Hypoxia can lead to liver fibrosis and severely limits the efficacy of photodynamic therapy (PDT). Herein, carbon nitride (CN)-based hybrid nanoparticles (NPs) VPSGCNs@TSI for light-driven water splitting were utilized to solve this problem. CNs were doped with selenide glucose (Se-glu) to enhance their red/NIR region absorption. Then, vitamin A-poly(ethylene glycol) (VA-PEG) fragments and aggregation-induced emission (AIE) photosensitizers TSI were introduced into Se-glu-doped CN NPs (VPSGCNs) to construct VPSGCNs@TSI NPs. The introduction of VA-PEG fragments enhanced the targeting of the NPs to activated hepatic stellate cells (HSCs) and reduced their toxicity to ordinary liver cells. VPSGCN units could trigger water splitting to generate O2 under 660 nm laser irradiation, improve the hypoxic environment of the fibrosis site, downregulate HIF-1α expression, and activate HSC ferroptosis via the HIF-1α/SLC7A11 pathway. In addition, generated O2 could also increase the reactive oxygen species (ROS) production of TSI units in a hypoxic environment, thereby completely reversing hypoxia-triggered PDT resistance to enhance the PDT effect. The combination of water-splitting materials and photodynamic materials showed a 1 + 1 > 2 effect in increasing oxygen levels in liver fibrosis, promoting ferroptosis of activated HSCs and reversing PDT resistance caused by hypoxia.


Assuntos
Ferroptose , Células Estreladas do Fígado , Cirrose Hepática , Nanopartículas , Fotoquimioterapia , Nanopartículas/química , Animais , Ferroptose/efeitos dos fármacos , Cirrose Hepática/tratamento farmacológico , Cirrose Hepática/patologia , Cirrose Hepática/metabolismo , Camundongos , Células Estreladas do Fígado/efeitos dos fármacos , Células Estreladas do Fígado/metabolismo , Células Estreladas do Fígado/patologia , Fármacos Fotossensibilizantes/farmacologia , Fármacos Fotossensibilizantes/química , Nitrilas/química , Nitrilas/farmacologia , Humanos , Hipóxia/tratamento farmacológico , Hipóxia/metabolismo , Espécies Reativas de Oxigênio/metabolismo
16.
Sci Total Environ ; 874: 162509, 2023 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-36870263

RESUMO

The environmental behavior of heavy metals in soil is significantly regulated by their binding with dissolved organic matter (DOM), which is affected by soil moisture contents. However, the mechanism of this interaction in soils with varying moisture is still not well understood. Using a combination of ultrafiltration, Cu(II) titration, and multispectral (ultraviolet-visible absorption, 3D fluorescence, Fourier transform infrared) analysis techniques, we studied the differences in the spectral characteristics and Cu(II) binding properties of soil dissolved organic matter (DOM) and its different molecular weight (MW) fractions with moisture gradients. We found that the abundance and spectral characters of soil DOM changed with increasing soil moisture, i.e., the increase in abundance while the decrease in aromaticity and humification index. The components of DOM, shown by Fluorescence region-integration (FRI) analysis, also changed, with an increase in the proportion of protein-like substances and a decrease of humic-like and fulvic-like substances. The overall Cu(II) binding potential of soil DOM diminished with increasing soil moisture, as indicated by the fluorescence parallel factor (PARAFAC) analysis. This is aligns with the changes in DOM composition, as the humic-like and fulvic-like fractions exhibited higher Cu(II) binding potential compared to the protein-like fractions. The low MW fraction of the MW-fractionated samples showed a stronger binding potential for Cu(II) compared to the high MW fraction. Finally, the active binding site of Cu(II) in DOM, as revealed by UV-difference spectroscopy and 2D-FTIR-COS analysis, decreased with increasing soil moisture, with the order of preferentially functional groups shifting from OH, NH, and CO to CN and CO. This study emphasizes the impact of moisture variations on the characteristics of DOM and its interaction with Cu(II), providing insight into the environmental fate of heavy metal contaminants in soil in areas with alternating land and water conditions.

17.
J Mater Chem B ; 11(14): 3186-3194, 2023 04 05.
Artigo em Inglês | MEDLINE | ID: mdl-36946887

RESUMO

Lipid droplets (LDs) and their autophagy by lysosomes are closely related to a variety of physiological and pathological conditions. Therefore, identifying and tracking LDs and the dynamic process of autophagy can provide useful information for the diagnostics and treatment of related diseases. However, few organic small molecule-based fluorescent probes can specifically recognize LDs and dynamically track their autophagy process. Herein, we synthesized a "discoloration" fluorescent bioprobe DPABP-BI with distinguishable features including red fluorescence emission (630 nm), large Stokes shift (145 nm), two-photon excitation and outstanding photostability and biocompatibility. In particular, LDs could be specifically identified via the red fluorescence emission of DPABP-BI (colocalization constant of 0.98), while autophagolysosomes could be visualized via the green fluorescence emission of its acid-hydrolyzed product (colocalization constant of 0.90) to track the autophagy dynamic process. In addition, DPABP-BI enabled the specific recognition of fatty substances in zebrafish larvae. In this study, a two-photon excited red light small molecule probe was constructed to identify LDs and track their autophagy dynamic process by changing the fluorescence emission wavelength.


Assuntos
Técnicas Biossensoriais , Gotículas Lipídicas , Animais , Peixe-Zebra , Lisossomos , Autofagia
18.
Sci Total Environ ; 873: 162246, 2023 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-36796690

RESUMO

The complexation of metals with dissolved organic matter (DOM) under different compositions and molecular weights (MWs) will result in different environmental fate and toxicity, but the specific role and impact of DOM MWs remain less well understood. This study explored the metal binding characteristics by DOM with different MWs from different sources, including sea, river, and wetland waters. The results of fluorescence characterization showed that the >1 kDa high-molecular-weight (HMW)-DOM were mainly from terrestrial sources while the low-molecular-weight (LMW)-DOM fractions were mostly from microbial sources. Based on UV-Vis spectroscopic characterization, the LMW-DOM contained more unsaturated bonds than its HMW counterpart, and the substituents are generally dominated by polar functional groups. Summer DOM had more unsaturated bonds and a higher metal binding capacity than winter DOM. Furthermore, DOM with different MWs had significantly different Cu binding properties. In addition, Cu binding with microbially derived LMW-DOM mainly caused the change in the peak at 280 nm, while binding with terrigenous HMW-DOM resulted in the change of the 210 nm peak. Compared with the HMW-DOM, most of the LMW-DOM had stronger Cu-binding ability. Correlation analysis indicates that metal binding ability of DOM mainly depends on its concentration, number of unsaturated bonds and benzene rings, and types of substituents during interactions. This work provides an improved understanding of the metal-DOM binding mechanism, the role of composition- and MW-dependent DOM from different sources, and thus the transformation and environmental/ecological role of metals in aquatic systems.

19.
Adv Sci (Weinh) ; 10(24): e2302358, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37350571

RESUMO

Designing and synthesizing advanced electrocatalysts with superior intrinsic activity toward hydrogen evolution reaction (HER) in alkaline media is critical for the hydrogen economy. Herein, a novel Ir@Rhene heterojunction electrocatalyst is synthesized via epitaxially confining ultrasmall and low-coordinate Ir nanoclusters on the ultrathin Rh metallene accompanying the formation of Ir/IrO2 Janus nanoparticles. The as-prepared heterojunctions display outstanding alkaline HER activity, with an overpotential of only 17 mV at 10 mA cm-2 and an ultralow Tafel slope of 14.7 mV dec-1 . Both structural characterizations and theoretical calculations demonstrate that the Ir@Rhene heterointerfaces induce charge density redistribution, resulting in the increment of the electron density around the O atoms in the IrO2 site and thus delivering much lower water dissociation energy. In addition, the dual-site synergetic effects between IrO2 and Ir/Rh interface trigger and improve the interfacial hydrogen spillover, thereby subtly avoiding the steric blocking of the active site and eventually accelerating the alkaline HER kinetics.

20.
Bioeng Transl Med ; 8(5): e10558, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37693059

RESUMO

High positive charge-induced toxicity, easy lysosomal degradation of nucleic acid drugs, and poor lesion sites targeting are major problems faced in the development of gene carriers. Herein, we proposed the concept of self-escape non-cationic gene carriers for targeted delivery and treatment of photocontrolled hepatocellular carcinoma (HCC) with sufficient lysosome escape and multiple response capacities. Functional DNA was bound to the surface of biotin-PEG2000-modified graphitic carbon nitride (Bio-PEG-CN) nanosheets to form non-cationic nanocomplexes Bio-PEG-CN/DNA. These nanocomposites could actively target HCC tissue. Once these nanocomplexes were taken up by tumor cells, the accumulated reactive oxygen species (ROS) generated by Bio-PEG-CN under LED irradiation would disrupt the lysosome structure, thereby facilitating nanocomposites escape. Due to the acidic microenvironment and lipase in the HCC tissue, the reversible release of DNA could be promoted to complete the transfection process. Meanwhile, the fluorescence signal of Bio-PEG-CN could be monitored in real time by fluorescence imaging technology to investigate the transfection process and mechanism. In vitro and in vivo results further demonstrated that these nanocomplexes could remarkably upregulate the expression of tumor suppressor protein P53, increased tumor sensitivity to ROS generated by nanocarriers, and realized effective gene therapy for HCC via loading P53 gene.

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