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1.
Angew Chem Int Ed Engl ; : e202408527, 2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38958191

RESUMO

Janus heterostructures consisting of multiple jointed components with distinct properties have gained growing interest in the photoredox catalytic field. Herein, we have developed a facile low-temperature method to gain anisotropic one-dimensional Au-tipped CdS (Au-CdS) nanorods (NRs), followed by assembling Ru molecular co-catalyst (RuN5) onto the surface of the NRs. The CdS NRs decorated with plasmonic Au nanoparticles (NPs) and RuN5 complex harness the virtues of metal-semiconductor and inorganic-organic interface, giving directional charge transfer channels, spatially separated reaction sites, and enhanced local electric field distribution. As a result, the Au-CdS-RuN5 can act as an efficient dual-function photocatalyst for simultaneous H2 evolution and valorization of biomass-derived alcohols. Benefiting from the interfacial charge decoupling and selective chemical bond activation, the optimal all-in-one Au-CdS-RuN5 heterostructure shows greatly enhanced photoactivity and selectivity as compared to bare CdS NRs, along with a remarkable apparent quantum yield of 40.2% at 400 nm. The structural evolution and working mechanism of the heterostructures are systematically analyzed based on experimental and computational results.

2.
Angew Chem Int Ed Engl ; : e202407791, 2024 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-38860734

RESUMO

Light-driven photoredox catalysis presents a promising approach for the activation and conversion of methane (CH4) into high value-added chemicals under ambient conditions. However, the high C-H bond dissociation energy of CH4 and the absence of well-defined C-H activation sites on catalysts significantly limit the highly efficient conversion of CH4 toward multicarbon (C2+) hydrocarbons, particularly ethylene (C2H4). Herein, we demonstrate a bimetallic design of Ag nanoparticles (NPs) and Pd single atoms (SAs) on ZnO for the cascade conversion of CH4 into C2H4 with the highest production rate compared with previous works. Mechanistic studies reveal that the synergistic effect of Ag NPs and Pd SAs, upon effecting key bond-breaking and -forming events, lowers the overall energy barrier of the activation process of both CH4 and the resulting C2H6, constituting a truly synergistic catalytic system to facilitate the C2H4 generation. This work offers a novel perspective on the advancement of photocatalytic directional CH4 conversion toward high value-added C2+ hydrocarbons through the subtle design of bimetallic cascade catalyst strategy.

3.
Nat Commun ; 15(1): 4880, 2024 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-38849347

RESUMO

Assembling graphene sheets into macroscopic fibers with graphitic layers uniaxially aligned along the fiber axis is of both fundamental and technological importance. However, the optimal performance of graphene-based fibers has been far lower than what is expected based on the properties of individual graphene. Here we show that both mechanical properties and electrical conductivity of graphene-based fibers can be significantly improved if bridges are created between graphene edges through covalent conjugating aromatic amide bonds. The improved electrical conductivity is likely due to extended electron conjugation over the aromatic amide bridged graphene sheets. The larger sheets also result in improved π-π stacking, which, along with the robust aromatic amide linkage, provides high mechanical strength. In our experiments, graphene edges were bridged using the established wet-spinning technique in the presence of an aromatic amine linker, which selectively reacts to carboxyl groups at the graphene edge sites. This technique is already industrial and can be easily upscaled. Our methodology thus paves the way to the fabrication of high-performance macroscopic graphene fibers under optimal techno-economic and ecological conditions.

4.
BMC Med Genomics ; 17(1): 137, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38778403

RESUMO

BACKGROUND: Head and neck squamous cell carcinoma (HNSCC) is a prevalent cancer with a poor survival rate due to anatomical limitations of the head and a lack of reliable biomarkers. Cuproptosis represents a novel cellular regulated death pathway, and N6-methyladenosine (m6A) is the most common internal RNA modification in mRNA. They are intricately connected to tumor formation, progression, and prognosis. This study aimed to construct a risk model for HNSCC using a set of mRNAs associated with m6A regulators and cuproptosis genes (mcrmRNA). METHODS: RNA-seq and clinical data of HNSCC patients from The Cancer Genome Atlas (TCGA) database were analyzed to develop a risk model through the least absolute shrinkage and selection operator (LASSO) analysis. Survival analysis and receiver operating characteristic (ROC) analysis were performed for the high- and low-risk groups. Additionally, the model was validated using the GSE41613 dataset from the Gene Expression Omnibus (GEO) database. GSEA and CIBERSORT were applied to investigate the immune microenvironment of HNSCC. RESULTS: A risk model consisting of 32 mcrmRNA was developed using the LASSO analysis. The risk score of patients was confirmed to be an independent prognostic indicator by multivariate Cox analysis. The high-risk group exhibited a higher tumor mutation burden. Additionally, CIBERSORT analysis indicated varying levels of immune cell infiltration between the two groups. Significant disparities in drug sensitivity to common medications were also observed. Enrichment analysis further unveiled significant differences in metabolic pathways and RNA processing between the two groups. CONCLUSIONS: Our risk model can predict outcomes for HNSCC patients and offers valuable insights for personalized therapeutic approaches.


Assuntos
Adenosina , Neoplasias de Cabeça e Pescoço , Carcinoma de Células Escamosas de Cabeça e Pescoço , Humanos , Carcinoma de Células Escamosas de Cabeça e Pescoço/genética , Carcinoma de Células Escamosas de Cabeça e Pescoço/patologia , Neoplasias de Cabeça e Pescoço/genética , Neoplasias de Cabeça e Pescoço/patologia , Adenosina/análogos & derivados , Adenosina/metabolismo , Masculino , RNA Mensageiro/genética , RNA Mensageiro/metabolismo , Prognóstico , Feminino , Biomarcadores Tumorais/genética , Medição de Risco , Regulação Neoplásica da Expressão Gênica , Pessoa de Meia-Idade , Microambiente Tumoral
5.
Artigo em Inglês | MEDLINE | ID: mdl-38753528

RESUMO

OBJECTIVES: Detection of early neoplastic lesions is crucial for improving the survival rates of patients with gastric cancer. Optical enhancement mode 2 is a new image-enhanced endoscopic technique that offers bright images and can improve the visibility of neoplastic lesions. This study aimed to compare the detection of neoplastic lesions with optical enhancement mode 2 and white-light imaging (WLI) in a high-risk population. METHODS: In this prospective multicenter randomized controlled trial, patients were randomly assigned to optical enhancement mode 2 or WLI groups. Detection of suspicious neoplastic lesions during the examinations was recorded, and pathological diagnoses served as the gold standard. RESULTS: A total of 1211 and 1219 individuals were included in the optical enhancement mode 2 and WLI groups, respectively. The detection rate of neoplastic lesions was significantly higher in the optical enhancement mode 2 group (5.1% vs. 1.9%; risk ratio, 2.656 [95% confidence interval, 1.630-4.330]; p < 0.001). The detection rate of neoplastic lesions with an atrophic gastritis background was significantly higher in the optical enhancement mode 2 group (8.6% vs. 2.6%, p < 0.001). The optical enhancement mode 2 group also had a higher detection rate among endoscopists with different experiences. CONCLUSIONS: Optical enhancement mode 2 was more effective than WLI for detecting neoplastic lesions in the stomach, and can serve as a new method for screening early gastric cancer in clinical practice. CLINICAL REGISTRY: United States National Library of Medicine (https://www. CLINICALTRIALS: gov), ID: NCT040720521.

6.
Redox Biol ; 72: 103140, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38593629

RESUMO

Gut microbiota has been implicated in the initiation and progression of various diseases; however, the underlying mechanisms remain elusive and effective therapeutic strategies are scarce. In this study, we investigated the role and mechanisms of gut microbiota in TNBS-induced colitis and its associated kidney injury while evaluating the potential of dietary protein as a therapeutic intervention. The intrarectal administration of TNBS induced colitis in mice, concurrently with kidney damage. Interestingly, this effect was absent when TNBS was administered intraperitoneally, indicating a potential role of gut microbiota. Depletion of gut bacteria with antibiotics significantly attenuated the severity of TNBS-induced inflammation, oxidative damage, and tissue injury in the colon and kidneys. Mechanistic investigations using cultured colon epithelial cells and bone-marrow macrophages unveiled that TNBS induced cell oxidation, inflammation and injury, which was amplified by the bacterial component LPS and mitigated by thiol antioxidants. Importantly, in vivo administration of thiol-rich whey protein entirely prevented TNBS-induced colonic and kidney injury. Our findings suggest that gut bacteria significantly contribute to the initiation and progression of colitis and associated kidney injury, potentially through mechanisms involving LPS-induced exaggeration of oxidative cellular damage. Furthermore, our research highlights the potential of dietary thiol antioxidants as preventive and therapeutic interventions.


Assuntos
Colite , Microbioma Gastrointestinal , Estresse Oxidativo , Ácido Trinitrobenzenossulfônico , Animais , Microbioma Gastrointestinal/efeitos dos fármacos , Estresse Oxidativo/efeitos dos fármacos , Colite/induzido quimicamente , Colite/microbiologia , Colite/metabolismo , Camundongos , Ácido Trinitrobenzenossulfônico/toxicidade , Ácido Trinitrobenzenossulfônico/efeitos adversos , Modelos Animais de Doenças , Masculino , Antioxidantes/farmacologia , Rim/metabolismo , Rim/patologia , Rim/efeitos dos fármacos
7.
ACS Appl Mater Interfaces ; 15(48): 55938-55947, 2023 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-37988589

RESUMO

Photoelectric devices are extensively applied in optical logic systems, light communication, optical imaging, and so on. However, traditional photoelectric devices can only generate unidirectional photocurrent, which hinders the simplification and multifunctionality of devices. Recently, it has become a new research focus to achieve controllable reversal of the output photocurrent direction (bipolar current) in a photoelectric system. Considering that the device with bipolar current adds a reverse current operating state compared to traditional devices, the former is more suitable for developing new multifunctional photoelectric devices. Due to the existence of electrolytes, photoelectrochemical (PEC) systems contain chemical processes such as ion diffusion and migration and electrochemical reactions, which are unable to occur in solid-state transistor devices, and the effect of electrolyte pH on the performance of PEC systems is usually ignored. We prepared a MnPS3-based PEC-type photodetector and reversed photocurrents by adjusting the pH of electrolytes, i.e., the electrolyte-controlled photoelectrochemical photocurrent switching (PEPS) effect. We clarified the effect of pH values on the direction of photocurrent from the perspectives of electrolyte energy level rearrangement splitting and the kinetic theory of the semiconductor electrode. This work not only contributes to a deeper understanding of carrier transport in PEC processes but also inspires the development of advanced multifunctional photoelectric devices.

8.
bioRxiv ; 2023 Nov 02.
Artigo em Inglês | MEDLINE | ID: mdl-37961182

RESUMO

The mammalian neocortex differs vastly in size and complexity between mammalian species, yet the mechanisms that lead to an increase in brain size during evolution are not known. We show here that two transcription factors coordinate gene expression programs in progenitor cells of the neocortex to regulate their proliferative capacity and neuronal output in order to determine brain size. Comparative studies in mice, ferrets and macaques demonstrate an evolutionary conserved function for these transcription factors to regulate progenitor behaviors across the mammalian clade. Strikingly, the two transcriptional regulators control the expression of large numbers of genes linked to microcephaly suggesting that transcriptional deregulation as an important determinant of the molecular pathogenesis of microcephaly, which is consistent with the finding that genetic manipulation of the two transcription factors leads to severe microcephaly. Summary: The neocortex varies in size and complexity among mammals due to the tremendous variability in the number and diversity of neuronal subtypes across species 1,2 . The increased cellular diversity is paralleled by the expansion of the pool of neocortical progenitors 2-5 and the emergence of indirect neurogenesis 6 during brain evolution. The molecular pathways that control these biological processes and are disrupted in neurological and psychiatric disorders remain largely unknown. Here we show that the transcription factors BRN1 (POU3F3) and BRN2 (POU3F2) act as master regulators of the transcriptional programs in progenitors linked to neuronal specification and neocortex expansion. Using genetically modified lissencephalic and gyrencephalic animals, we found that BRN1/2 establish transcriptional programs in neocortical progenitors that control their proliferative capacity and the switch from direct to indirect neurogenesis. Functional studies in genetically modified mice and ferrets show that BRN1/2 act in concert with NOTCH and primary microcephaly genes to regulate progenitor behavior. Analysis of transcriptomics data from genetically modified macaques provides evidence that these molecular pathways are conserved in non-human primates. Our findings thus establish a mechanistic link between BRN1/2 and genes linked to microcephaly and demonstrate that BRN1/2 are central regulators of gene expression programs in neocortical progenitors critical to determine brain size during evolution.

9.
Thorac Cancer ; 14(25): 2579-2590, 2023 09.
Artigo em Inglês | MEDLINE | ID: mdl-37548102

RESUMO

BACKGROUND: Histone methyltransferases are crucial regulators in non-small cell lung cancer (NSCLC) development. This study explored the mechanism of histone methyltransferase SET domain containing 1A (SETD1A)-mediated H3K4me2 methylation in NSCLC cell ferroptosis and provides novel targets for NSCLC treatment. METHODS: Upon downregulation of SETD1A in NSCLC cell lines, cell proliferation potential, malondialdehyde (MDA), superoxide dismutase (SOD) and glutathione (GSH) activities, iron content, and SETD1A, long noncoding RNA HOXC cluster antisense RNA 3 (lncRNA HOXC-AS3), E1A binding protein p300 (EP300), glutathione peroxidase 4 (GPX4) expressions were determined via cell counting kit-8, ELISA, iron assay kits, RT-qPCR, and western blot. Enrichment levels of SETD1A and H3K4me3 in the HOXC-AS3 promotor were measured via chromatin immunoprecipitation, and the binding of HOXC-AS3 and EP300 was analyzed via RNA immunoprecipitation. Rescue experiments were performed to confirm their roles in NSCLC cell ferroptosis. Xenograft tumor models were established to validate the role of SETD1A in vivo. RESULTS: SETD1A, H3K4me3, HOXC-AS3, and EP300 were highly-expressed in NSCLC cells. Silencing SETD1A inhibited NSCLC cell proliferation, increased MDA and iron levels, and decreased SOD, GSH, and GPX4 levels. SETD1A downregulation reduced H3K4me3 level, HOXC-AS3 expression, the binding of HOXC-AS3 to EP300, and EP300 stability. Overexpression of HOXC-AS3 or EP300 reversed the promotion of silencing SETD1A on NSCLC cell ferroptosis. Silencing SETD1A reduced tumor volume and weight and positive rate of ki67 and increased ferroptosis through the HOXC-AS3/EP300 axis. CONCLUSION: SETD1A-mediated H3K4me2 methylation promoted HOXC-AS3 expression, binding of HOXC-AS3 to EP300, and EP300 stability, thereby suppressing NSCLC cell ferroptosis.


Assuntos
Carcinoma Pulmonar de Células não Pequenas , Ferroptose , Neoplasias Pulmonares , RNA Longo não Codificante , Humanos , Carcinoma Pulmonar de Células não Pequenas/patologia , RNA Longo não Codificante/genética , Neoplasias Pulmonares/patologia , Metilação , Linhagem Celular Tumoral , Proliferação de Células/genética , Proteína p300 Associada a E1A/metabolismo
10.
Angew Chem Int Ed Engl ; 62(41): e202311731, 2023 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-37632151

RESUMO

Solar-driven CO2 reduction integrated with C-C/C-X bond-forming organic synthesis represents a substantially untapped opportunity to simultaneously tackle carbon neutrality and create an atom-/redox-economical chemical synthesis. Herein, we demonstrate the first cooperative photoredox catalysis of efficient and tunable CO2 reduction to syngas, paired with direct alkylation/arylation of unactivated allylic sp3 C-H bonds for accessing allylic C-C products, over SiO2 -supported single Ni atoms-decorated CdS quantum dots (QDs). Our protocol not only bypasses additional oxidant/reductant and pre-functionalization of organic substrates, affording a broad of allylic C-C products with moderate to excellent yields, but also produces syngas with tunable CO/H2 ratios (1 : 2-5 : 1). Such win-win coupling catalysis highlights the high atom-, step- and redox-economy, and good durability, illuminating the tantalizing possibility of a renewable sunlight-driven chemical feedstocks manufacturing industry.

11.
Chem Soc Rev ; 52(15): 5013-5050, 2023 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-37431250

RESUMO

The ubiquity of solid-liquid interfaces in nature and the significant role of their atomic-scale structure in determining interfacial properties have led to intensive research. Particularly in electrocatalysis, however, a molecular-level picture that clearly describes the dynamic interfacial structures and organizations with their correlation to preferred reaction pathways in electrochemical reactions remains poorly understood. In this review, CO2 electroreduction reaction (CO2RR) is spatially and temporally understood as a result of intricate interactions at the interface, in which the interfacial features are highly relevant. We start with the discussion of current understandings and model development associated with the charged electrochemical interface as well as its dynamic landscape. We further highlight the interactive dynamics from the interfacial field, catalyst surface charges and various gradients in electrolyte and interfacial water structures at interfaces under CO2RR working conditions, with emphasis on the interfacial-structure dependence of catalytic reactivity/selectivity. Significantly, a probing energy-dependent "in situ characterization map" for dynamic interfaces based on various complementary in situ/operando techniques is proposed, aiming to present a comprehensive picture of interfacial electrocatalysis and to provide a more unified research framework. Moreover, recent milestones in both experimental and theoretical aspects to establish the correct profile of electrochemical interfaces are stressed. Finally, we present key scientific challenges with related perspectives toward future opportunities for this exciting frontier.

12.
Mol Cancer ; 22(1): 91, 2023 06 01.
Artigo em Inglês | MEDLINE | ID: mdl-37264402

RESUMO

Cancer therapy resistance is the main cause of cancer treatment failure. The mechanism of therapy resistance is a hot topic in epigenetics. As one of the most common RNA modifications, N6-methyladenosine (m6A) is involved in various processes of RNA metabolism, such as stability, splicing, transcription, translation, and degradation. A large number of studies have shown that m6A RNA methylation regulates the proliferation and invasion of cancer cells, but the role of m6A in cancer therapy resistance is unclear. In this review, we summarized the research progress related to the role of m6A in regulating therapy resistance in cancers.


Assuntos
Neoplasias , Humanos , Metilação , Neoplasias/tratamento farmacológico , Neoplasias/genética , Neoplasias/metabolismo , Splicing de RNA , Epigênese Genética , RNA/metabolismo
13.
Entropy (Basel) ; 25(6)2023 May 26.
Artigo em Inglês | MEDLINE | ID: mdl-37372201

RESUMO

Unpaired single-image dehazing has become a challenging research hotspot due to its wide application in modern transportation, remote sensing, and intelligent surveillance, among other applications. Recently, CycleGAN-based approaches have been popularly adopted in single-image dehazing as the foundations of unpaired unsupervised training. However, there are still deficiencies with these approaches, such as obvious artificial recovery traces and the distortion of image processing results. This paper proposes a novel enhanced CycleGAN network with an adaptive dark channel prior for unpaired single-image dehazing. First, a Wave-Vit semantic segmentation model is utilized to achieve the adaption of the dark channel prior (DCP) to accurately recover the transmittance and atmospheric light. Then, the scattering coefficient derived from both physical calculations and random sampling means is utilized to optimize the rehazing process. Bridged by the atmospheric scattering model, the dehazing/rehazing cycle branches are successfully combined to form an enhanced CycleGAN framework. Finally, experiments are conducted on reference/no-reference datasets. The proposed model achieved an SSIM of 94.9% and a PSNR of 26.95 on the SOTS-outdoor dataset and obtained an SSIM of 84.71% and a PSNR of 22.72 on the O-HAZE dataset. The proposed model significantly outperforms typical existing algorithms in both objective quantitative evaluation and subjective visual effect.

14.
Mar Biotechnol (NY) ; 25(3): 463-472, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37289264

RESUMO

Isochrysis zhangjiangensis is an important microalgal species used as bait in aquaculture. However, its optimal cultivation temperature is around 25 °C, limiting its use in summer when temperature is higher. To overcome this limitation, we aimed to develop a consortia of I. zhangjiangensis and bacteria that are more resistant to heat stress. Here, six thermotolerance-promoting bacterial strains were isolated from the culture of a heat-tolerant mutant strain of I. zhangjiangensis (IM), and identified as Algoriphagus marincola, Nocardioides sp., Pseudidiomarina sp., Labrenzia alba, Nitratireductor sp., and Staphylococcus haemolyticus. Further, co-culturing I. zhangjiangensis with A. marincola under high temperature conditions increased cell density, chlorophyll a, PSII maximum photochemical efficiency (Fv/Fm), and soluble protein content of microalgae. The presence of A. marincola positively influenced the activities of superoxide dismutase (SOD), peroxidase (POD), catalase (CAT), and total antioxidant capacity (T-AOC) in I. zhangjiangensis cells, while concurrently reducing the levels of reactive oxygen species (ROS). Additionally, gene expression studies confirmed that co-culturing with A. marincola upregulated the expression of antioxidant-related genes (sod and pod) and stress tolerance genes (heat shock protein genes). Our findings indicate that A. marincola effectively helps I. zhangjiangensis withstand high temperature stress, leading to improved yield of microalgae during high temperature conditions. The thermotolerance-promoting bacteria can be exploited as potential inoculants for enhancing the productivity and sustainability of bait microalgae in aquaculture.


Assuntos
Haptófitas , Termotolerância , Antioxidantes/metabolismo , Haptófitas/metabolismo , Clorofila A/metabolismo , Bactérias
15.
Angew Chem Int Ed Engl ; 62(29): e202304306, 2023 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-37208951

RESUMO

Benzimidazoles are a versatile class of scaffolds with important biological activities, whereas their synthesis in a lower-cost and more efficient manner remains a challenge. Here, we demonstrate a conceptually new radical route for the high-performance photoredox coupling of alcohols and diamines to synthesize benzimidazoles along with stoichiometric hydrogen (H2 ) over Pd-decorated ultrathin ZnO nanosheets (Pd/ZnO NSs). The mechanistic study reveals the unique advantage of ZnO NSs over other supports and particularly that the features of Pd nanoparticles in facilitating the cleavage of the α-C-H bond of alcohols and adsorbing subsequently-generated C-centered radicals hold the key to turning on the reaction. This work highlights a new insight into radical-induced efficient benzimidazole synthesis pairing with H2 evolution by rationally designing semiconductor-based photoredox systems.

16.
Front Neurol ; 14: 1100469, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36908598

RESUMO

Objective: This systematic review was performed to identify the role of cognitive reserve (CR) proxies in the functional outcome and mortality prognostication of patients after acute ischemic stroke. Methods: PubMed, Embase, Web of Science, and Cochrane Library were comprehensively searched by two independent reviewers from their inception to 31 August 2022, with no restrictions on language. The reference lists of reviews or included articles were also searched. Cohort studies with a follow-up period of ≥3 months identifying the association between CR indicators and the post-stroke functional outcome and mortality were included. The outcome records for patients with hemorrhage and ischemic stroke not reported separately were excluded. The Quality In Prognosis Studies (QUIPS) tool was used to assess the quality of included studies. Results: Our search yielded 28 studies (n = 1,14,212) between 2004 and 2022, of which 14 were prospective cohort studies and 14 were retrospective cohort studies. The follow-up period ranged from 3 months to 36 years, and the mean or median age varied from 39.6 to 77.2 years. Of the 28 studies, 15 studies used the functional outcome as their primary outcome interest, and 11 of the 28 studies included the end-point interest of mortality after ischemic stroke. In addition, two of the 28 studies focused on the interest of functional outcomes and mortality. Among the included studies, CR proxies were measured by education, income, occupation, premorbid intelligence quotient, bilingualism, and socioeconomic status, respectively. The quality of the review studies was affected by low to high risk of bias. Conclusion: Based on the current literature, patients with ischemic stroke with higher CR proxies may have a lower risk of adverse outcomes. Further prospective studies involving a combination of CR proxies and residuals of fMRI measurements are warranted to determine the contribution of CR to the adverse outcome of ischemic stroke. Systematic review registration: PROSPERO, identifier CRD42022332810, https://www.crd.york.ac.uk/PROSPERO/.

17.
Research (Wash D C) ; 6: 0073, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36930756

RESUMO

Semiconductor quantum dots have been emerging as one of the most ideal materials for artificial photosynthesis. Here, we report the assembled ZnS-CdS hybrid heterostructure for efficient coupling cooperative redox catalysis toward the oxidation of 1-phenylethanol to acetophenone/2,3-diphenyl-2,3-butanediol (pinacol) integrated with the reduction of protons to H2. The strong interaction and typical type-I band-position alignment between CdS quantum dots and ZnS quantum dots result in efficient separation and transfer of electron-hole pairs, thus distinctly enhancing the coupled photocatalyzed-redox activity and stability. The optimal ZnS-CdS hybrid also delivers a superior performance for various aromatic alcohol coupling photoredox reaction, and the ratio of electrons and holes consumed in such redox reaction is close to 1.0, indicating a high atom economy of cooperative coupling catalysis. In addition, by recycling the scattered light in the near field of a SiO2 sphere, the SiO2-supported ZnS-CdS (denoted as ZnS-CdS/SiO2) catalyst can further achieve a 3.5-fold higher yield than ZnS-CdS hybrid. Mechanistic research clarifies that the oxidation of 1-phenylethanol proceeds through the pivotal radical intermediates of •C(CH3)(OH)Ph. This work is expected to promote the rational design of semiconductor quantum dots-based heterostructured catalysts for coupling photoredox catalysis in organic synthesis and clean fuels production.

18.
Angew Chem Int Ed Engl ; 62(22): e202303054, 2023 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-36988009

RESUMO

Photocatalytic epoxide alcoholysis through C-O bond cleavage and formation has emerged as an alternative to synthesizing anti-tumoral pharmaceuticals and fine chemicals. However, the lack of crucial evidence to interpret the interaction between reactants and photocatalyst surface makes it challenging for photocatalytic epoxide alcoholysis with both high activity and regioselectivity. In this work, we report the hierarchical ZnIn2 S4 @CdS photocatalyst for epoxide alcoholysis with high regioselectivity nearly 100 %. Mechanistic studies unveil that the precise activation switch on exposed Zn acid sites for C-O bond polarization and cleavage has a critical significance for achieving efficient photocatalytic performance. Furthermore, the establishment of Z-scheme heterojunction facilitates the interface charge separation and transfer. Remarkably, the underlying regioselective photocatalytic reaction pathway has been distinctly revealed.

19.
iScience ; 26(3): 106177, 2023 Mar 17.
Artigo em Inglês | MEDLINE | ID: mdl-36895655

RESUMO

As an elemental semiconductor, tellurium (Te) has been famous for its high hole-mobility, excellent ambient stability and topological states. Here, we realize the controllable synthesis of horizontal Te nanoribbon arrays (TRAs) with an angular interval of 60°on mica substrates by physical vapor deposition strategy. The growth of Te nanoribbons (TRs) is driven by two factors, where the intrinsic quasi-one-dimensional spiral chain structure promotes the elongation of their length; the epitaxy relationship between [110] direction of Te and [110] direction of mica facilitates the oriented growth and the expansion of their width. The bending of TRs which have not been reported is induced by grain boundary. Field-effect transistors based on TRs demonstrate high mobility and on/off ratio corresponding to 397 cm2 V-1 s-1 and 1.5×105, respectively. These phenomena supply an opportunity to deep insight into the vapor-transport synthesis of low-dimensional Te and explore its underlying application in monolithic integration.

20.
Front Endocrinol (Lausanne) ; 14: 1077059, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36896178

RESUMO

Objective: By studying the changes of serum uric acid (SUA) in acute stage and remission stage of gouty arthritis, we aimed to explore the relationship between the changes of SUA level and free glucocorticoids and inflammatory factors. Methods: A prospective, longitudinal study was conducted on 50 acute gout patients in the dedicated gout clinic of the Affiliated Hospital of Qingdao University. Blood and 24-hour urine samples were collected during the acute phase and two weeks after the initial visit. Patients with acute gouty arthritis were treated primarily with colchicine and nonsteroidal anti-inflammatory drugs. Results: A total of 32 patients completed the two-week follow-up trial. SUA levels were significantly downregulated during the acute flare than after the flare (464.14 ± 90.97 vs. 527.36 ± 86.90 µmol/L, p < 0.001). The 24-hour fractional excretion of uric acid (24 h FEur) (5.54 ± 2.82% vs. 4.68 ± 2.83%, p < 0.001) and 24-hour urinary uric acid excretion (24 h Uur) (663.08 ± 249.48 µmol/L vs. 540.87 ± 263.18 µmol/L, p = 0.001) increased significantly in patients during the acute phase. The percent change in SUA was associated with those in 24 h FEur and C-reactive protein. Meanwhile, the percent change in 24 h Uur was associated with those in 24-hour urinary free cortisol, percent change in interleukin 1ß and interleukin 6. Conclusion: Decreased SUA level during the acute gout flare was associated with increased excretion of urinary uric acid. Inflammatory factors and bioactive free glucocorticoids may play significant roles in this process.


Assuntos
Artrite Gotosa , Gota , Humanos , Artrite Gotosa/tratamento farmacológico , Ácido Úrico , Estudos Prospectivos , Estudos Longitudinais , Exacerbação dos Sintomas
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