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1.
Nature ; 625(7995): 516-522, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-38233617

RESUMO

Perovskite solar cells (PSCs) comprise a solid perovskite absorber sandwiched between several layers of different charge-selective materials, ensuring unidirectional current flow and high voltage output of the devices1,2. A 'buffer material' between the electron-selective layer and the metal electrode in p-type/intrinsic/n-type (p-i-n) PSCs (also known as inverted PSCs) enables electrons to flow from the electron-selective layer to the electrode3-5. Furthermore, it acts as a barrier inhibiting the inter-diffusion of harmful species into or degradation products out of the perovskite absorber6-8. Thus far, evaporable organic molecules9,10 and atomic-layer-deposited metal oxides11,12 have been successful, but each has specific imperfections. Here we report a chemically stable and multifunctional buffer material, ytterbium oxide (YbOx), for p-i-n PSCs by scalable thermal evaporation deposition. We used this YbOx buffer in the p-i-n PSCs with a narrow-bandgap perovskite absorber, yielding a certified power conversion efficiency of more than 25%. We also demonstrate the broad applicability of YbOx in enabling highly efficient PSCs from various types of perovskite absorber layer, delivering state-of-the-art efficiencies of 20.1% for the wide-bandgap perovskite absorber and 22.1% for the mid-bandgap perovskite absorber, respectively. Moreover, when subjected to ISOS-L-3 accelerated ageing, encapsulated devices with YbOx exhibit markedly enhanced device stability.

2.
Plant Physiol ; 192(4): 2737-2755, 2023 08 03.
Artigo em Inglês | MEDLINE | ID: mdl-37086480

RESUMO

Magnesium chelatase (MgCh) catalyzes the insertion of magnesium into protoporphyrin IX, a vital step in chlorophyll (Chl) biogenesis. The enzyme consists of 3 subunits, MgCh I subunit (CHLI), MgCh D subunit (CHLD), and MgCh H subunit (CHLH). The CHLI subunit is an ATPase that mediates catalysis. Previous studies on CHLI have mainly focused on model plant species, and its functions in other species have not been well described, especially with regard to leaf coloration and metabolism. In this study, we identified and characterized a CHLI mutant in strawberry species Fragaria pentaphylla. The mutant, noted as p240, exhibits yellow-green leaves and a low Chl level. RNA-Seq identified a mutation in the 186th amino acid of the CHLI subunit, a base conserved in most photosynthetic organisms. Transient transformation of wild-type CHLI into p240 leaves complemented the mutant phenotype. Further mutants generated from RNA-interference (RNAi) and CRISPR/Cas9 gene editing recapitulated the mutant phenotype. Notably, heterozygous chli mutants accumulated more Chl under low light conditions compared with high light conditions. Metabolite analysis of null mutants under high light conditions revealed substantial changes in both nitrogen and carbon metabolism. Further analysis indicated that mutation in Glu186 of CHLI does not affect its subcellular localization nor the interaction between CHLI and CHLD. However, intramolecular interactions were impaired, leading to reduced ATPase and MgCh activity. These findings demonstrate that Glu186 plays a key role in enzyme function, affecting leaf coloration via the formation of the hexameric ring itself, and that manipulation of CHLI may be a means to improve strawberry plant fitness and photosynthetic efficiency under low light conditions.


Assuntos
Fragaria , Liases , Mutação Puntual , Fragaria/genética , Fragaria/metabolismo , Liases/genética , Liases/metabolismo , Mutação/genética , Adenosina Trifosfatases/metabolismo , Folhas de Planta/genética , Folhas de Planta/metabolismo , Clorofila/metabolismo
3.
Gastrointest Endosc ; 99(2): 155-165.e4, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37820930

RESUMO

BACKGROUND AND AIMS: The lack of tissue traction and instrument dexterity to allow for adequate visualization and effective dissection were the main issues in performing endoscopic submucosal dissection (ESD). Robot-assisted systems may provide advantages. In this study we developed a novel transendoscopic telerobotic system and evaluated its performance in ESD. METHODS: A miniature dual-arm robotic endoscopic assistant for minimally invasive surgery (DREAMS) was developed. The DREAMS system contained the current smallest robotic ESD instruments and was compatible with the commercially available dual-channel endoscope. After the system was established, a prospective randomized controlled study was conducted to validate the performance of the DREAMS-assisted ESD in terms of efficacy, safety, and workload by comparing it with the conventional technique. RESULTS: Two robotic instruments can achieve safe collaboration and provide sufficient visualization and efficient dissection during ESD. Forty ESDs in the stomach and esophagus of 8 pigs were completed by DREAMS-assisted ESD or conventional ESD. Submucosal dissection time was comparable between the 2 techniques, but DREAMS-assisted ESD demonstrated a significantly lower muscular injury rate (15% vs 50%, P = .018) and workload scores (22.30 vs 32.45, P < .001). In the subgroup analysis of esophageal ESD, DREAMS-assisted ESD showed significantly improved submucosal dissection time (6.45 vs 16.37 minutes, P = .002), muscular injury rate (25% vs 87.5%, P = .041), and workload (21.13 vs 40.63, P = .001). CONCLUSIONS: We developed a novel transendoscopic telerobotic system, named DREAMS. The safety profile and technical feasibility of ESD were significantly improved with the assistance of the DREAMS system, especially in the narrower esophageal lumen.


Assuntos
Ressecção Endoscópica de Mucosa , Procedimentos Cirúrgicos Robóticos , Animais , Ressecção Endoscópica de Mucosa/instrumentação , Ressecção Endoscópica de Mucosa/métodos , Esôfago/cirurgia , Estudos Prospectivos , Estômago/cirurgia , Suínos , Resultado do Tratamento , Procedimentos Cirúrgicos Robóticos/instrumentação , Procedimentos Cirúrgicos Robóticos/métodos
4.
Environ Sci Technol ; 58(18): 7826-7837, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38653213

RESUMO

The interaction effects between the main components (proteins (P), carbohydrates (C), and lipids (L)) of protein-rich biomass during microwave-assisted pyrolysis were investigated in depth with an exploration of individual pyrolysis and copyrolysis (PC, PL, and CL) of model compounds. The average heating rate of P was higher than those of C and L, and the interactions in all copyrolysis groups reduced the max instant heating rate. The synergistic extent (S) of PC and PL for bio-oil yield was 16.78 and 18.24%, respectively, indicating that the interactions promoted the production of bio-oil. Besides, all of the copyrolysis groups exhibited a synergistic effect on biochar production (S = 19.43-28.24%), while inhibiting the gas generation, with S ranging from -20.17 to -6.09%. Regarding the gaseous products, apart from H2, P, C, and L primarily generated CO2, CO, and CH4, respectively. Regarding bio-oil composition, the interactions occurring within PC, PL, and CL exhibited a significantly synergistic effect (S = 47.81-412.96%) on the formation of N-heterocyclics/amides, amides/nitriles, and acids/esters, respectively. Finally, the favorable applicability of the proposed interaction effects was verified with microalgae. This study offers valuable insights for understanding the microwave-assisted pyrolysis of protein-rich biomass, laying the groundwork for further research and process optimization.


Assuntos
Biomassa , Micro-Ondas , Pirólise , Proteínas/química , Lipídeos/química , Carvão Vegetal/química , Carboidratos/química , Biocombustíveis
5.
J Biopharm Stat ; : 1-13, 2024 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-38515248

RESUMO

There is growing interest in understanding geographic patterns of medical device-related adverse events (AEs). A spatial scan method combined with the likelihood ratio test (LRT) for spatial-cluster signal detection over the geographical region is universally used. The spatial scan method used a moving window to scan the entire study region and collected some candidate sub-regions from which the spatial-cluster signal(s) will be found. However, it has some challenges, especially in computation. First, the computational cost increased when the number of sub-regions increased. Second, the computational cost may increase if a large spatial-cluster pattern is present and a flexible-shaped window is used. To reduce the computational cost, we propose a Bayesian nonparametric method that combines the ideas of Markov random field (MRF) to leverage geographical information to find potential signal clusters. Then, the LRT is applied for the detection of spatial cluster signals. The proposed method provides an ability to capture both locally spatially contiguous clusters and globally discontiguous clusters, and is manifested to be effective and tractable using hypothetical Left Ventricular Assist Device (LVAD) data as an illustration.

6.
Proc Natl Acad Sci U S A ; 118(8)2021 02 23.
Artigo em Inglês | MEDLINE | ID: mdl-33593897

RESUMO

Most eukaryotes possess two RecA-like recombinases (ubiquitous Rad51 and meiosis-specific Dmc1) to promote interhomolog recombination during meiosis. However, some eukaryotes have lost Dmc1. Given that mammalian and yeast Saccharomyces cerevisiae (Sc) Dmc1 have been shown to stabilize recombination intermediates containing mismatches better than Rad51, we used the Pezizomycotina filamentous fungus Trichoderma reesei to address if and how Rad51-only eukaryotes conduct interhomolog recombination in zygotes with high sequence heterogeneity. We applied multidisciplinary approaches (next- and third-generation sequencing technology, genetics, cytology, bioinformatics, biochemistry, and single-molecule biophysics) to show that T. reesei Rad51 (TrRad51) is indispensable for interhomolog recombination during meiosis and, like ScDmc1, TrRad51 possesses better mismatch tolerance than ScRad51 during homologous recombination. Our results also indicate that the ancestral TrRad51 evolved to acquire ScDmc1-like properties by creating multiple structural variations, including via amino acid residues in the L1 and L2 DNA-binding loops.


Assuntos
Proteínas de Ciclo Celular/metabolismo , Proteínas de Ligação a DNA/metabolismo , Proteínas Fúngicas/metabolismo , Genoma Fúngico , Recombinação Homóloga , Hypocreales/metabolismo , Meiose , Rad51 Recombinase/metabolismo , Proteínas de Saccharomyces cerevisiae/metabolismo , Proteínas de Ciclo Celular/genética , DNA de Cadeia Simples , Proteínas de Ligação a DNA/genética , Proteínas Fúngicas/genética , Hypocreales/genética , Rad51 Recombinase/genética , Saccharomyces cerevisiae/genética , Saccharomyces cerevisiae/metabolismo , Proteínas de Saccharomyces cerevisiae/genética
7.
J Am Chem Soc ; 145(49): 27054-27066, 2023 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-38040669

RESUMO

Single-atom catalysts (SACs) featuring M-N-C moieties have garnered significant attention as efficient electrocatalysts for the oxygen reduction reaction (ORR). However, the role of the dynamic M-N configuration of SACs induced by the derived frameworks under applied ORR potentials remains poorly understood. Herein, we conduct a comprehensive investigation using multiple operando techniques to assess the dynamic configurations of Cu SACs under various microstructural interface (MSI) regulations by anchoring atomic Cu on g-C3N4 and zeolitic imidazolate framework (ZIF) substrates. Cu SACs supported on g-C3N4 exhibit symmetric Cu-N configurations characterized by a reversibly adaptive nature under operational conditions, which leads to their excellent ORR catalytic activity. In contrast, the Cu-N configuration in ZIF-derived Cu SACs undergoes irreversible structural changes during the ORR process, in which the elongated Cu-N pair is unstable and breaks during the ORR, acting as a competing reaction against the ORR and resulting in high overpotential requirements. Crucially, operando time-resolved X-ray absorption spectroscopy (TR-XAS) and Raman results unequivocally reveal the reversibly adapting properties of the local Cu-N configuration in atomic Cu-anchored g-C3N4, which have been overlooked in numerous literatures. All findings provide valuable insights into the potential-driven characteristics of atomic electrocatalysts during target reactions and offer a systematic approach to study atomic electrocatalysts and their corresponding catalytic behaviors.

8.
Opt Express ; 31(2): 1103-1111, 2023 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-36785152

RESUMO

In this article, a compact racetrack double microring resonator (MRR) sensor based on Ge28Sb12Se60 (GeSbSe) is investigated. The sensor device consists of a racetrack microring, an embedded small microring, and a strip waveguide. Electron beam lithography (EBL) and dry etching are used to fabricate the device. The compact racetrack double MRR device are obtained with Q-factor equal to 7.17 × 104 and FSR of 24 nm by measuring the transmission spectrum. By measuring different concentrations of glucose solutions, a sensitivity of 297 nm/RIU by linear fitting and an intrinsic limit of detection (iLOD) of 7.40 × 10-5 are obtained. It paves the way for the application of chalcogenide glasses in the field of biosensing.

9.
Opt Express ; 31(20): 33403-33404, 2023 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-37859123

RESUMO

We correct the error in [Opt. Express31, 1103(2023)10.1364/OE.478613] Fig. 5(c). The unit of the vertical axis in the figure should be arbitrary units, not dB. All the conclusions are not changed after the correction.

10.
Plant Cell ; 32(4): 904-922, 2020 04.
Artigo em Inglês | MEDLINE | ID: mdl-31988264

RESUMO

Exon junction complexes (EJCs) are deposited on mRNAs during splicing and displaced by ribosomes during the pioneer round of translation. Nonsense-mediated mRNA decay (NMD) degrades EJC-bound mRNA, but the lack of suitable methodology has prevented the identification of other degradation pathways. Here, we show that the RNA degradomes of Arabidopsis (Arabidopsis thaliana), rice (Oryza sativa), worm (Caenorhabditis elegans), and human (Homo sapiens) cells exhibit an enrichment of 5' monophosphate (5'P) ends of degradation intermediates that map to the canonical EJC region. Inhibition of 5' to 3' exoribonuclease activity and overexpression of an EJC disassembly factor in Arabidopsis reduced the accumulation of these 5'P ends, supporting the notion that they are in vivo EJC footprints. Hundreds of Arabidopsis NMD targets possess evident EJC footprints, validating their degradation during the pioneer round of translation. In addition to premature termination codons, plant microRNAs can also direct the degradation of EJC-bound mRNAs. However, the production of EJC footprints from NMD but not microRNA targets requires the NMD factor SUPPRESSOR WITH MORPHOLOGICAL EFFECT ON GENITALIA PROTEIN7. Together, our results demonstrating in vivo EJC footprinting in Arabidopsis unravel the composition of the RNA degradome and provide a new avenue for studying NMD and other mechanisms targeting EJC-bound mRNAs for degradation before steady state translation.


Assuntos
Éxons/genética , Biossíntese de Proteínas/genética , Estabilidade de RNA/genética , Regiões 3' não Traduzidas/genética , Arabidopsis/genética , Proteínas de Arabidopsis/genética , Proteínas de Arabidopsis/metabolismo , Códon sem Sentido/genética , Exorribonucleases/metabolismo , Genes de Plantas , MicroRNAs/genética , MicroRNAs/metabolismo , Degradação do RNAm Mediada por Códon sem Sentido/genética , Oryza/genética
11.
Am J Hematol ; 98(11): 1742-1750, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37647123

RESUMO

Marginal zone lymphoma (MZL) is an indolent type of non-Hodgkin lymphoma that develops through pathological B cell receptor signaling. Orelabrutinib, a new-generation oral small molecule Bruton's tyrosine kinase inhibitor, was evaluated in relapsed/refractory (r/r) MZL patients. Previously treated r/r MZL patients received orelabrutinib 150 mg once daily in a phase 2, multicenter, single-arm study conducted in China. The primary endpoint was overall response rate (ORR) assessed by an Independent Review Committee (IRC) based on the Lugano 2014 classification. Other efficacy, safety, and pharmacokinetic profiles were evaluated as secondary outcome measures. A total of 111 patients were enrolled, of which 90 patients had MZL confirmed by central pathology review, who were mainly with extra-nodal MZL of mucosa-associated lymphoid tissue (MALT, 46.7%) and nodal MZL (35.6%). The majority had late-stage disease, with stage IV accounting for 75.6%. After a median follow-up duration of 24.3 months, the IRC-assessed ORR was 58.9% (95% confidence interval [CI], 48.0-69.2), with rates of complete response and partial response being 11.1% and 47.8%, respectively. The IRC-assessed median duration of response was 34.3 months, and the IRC-assessed median progression-free survival (PFS) was not reached with a 12-month PFS rate of 82.8% (95% CI, 72.6-89.5). The rate of overall survival at 12 months was 91.0% (95% CI, 82.8-95.4). Common all-grade treatment-related adverse events (TRAEs) included anemia (27.9%), neutrophil count decrease (23.4%), white blood cell count decrease (18.0%), platelet count decrease (17.1%), blood present in urine (16.2%), rash (14.4%), and upper respiratory tract infection (10.8%). Thirty-four patients (30.6%) experienced grade 3 or higher TRAEs. Serious TRAEs occurred in 18 patients (16.2%), of which pneumonia (5.4%) was the most common. Seven patients (6.3%) discontinued orelabrutinib due to TRAEs. Orelabrutinib demonstrated high response rates with durable disease remission and was well tolerated in Chinese patients with r/r MZL.

12.
Mod Rheumatol ; 33(1): 207-216, 2023 Jan 03.
Artigo em Inglês | MEDLINE | ID: mdl-34932796

RESUMO

OBJECTIVES: This retrospective cohort study aimed to find out predictors and early biomarkers of Infliximab (IFX) refractory intestinal Behçet's syndrome (intestinal BS). METHODS: We collected the baseline clinical characteristics, laboratory parameters, and concomitant therapies of intestinal BS patients treated by IFX from the Shanghai Behçet's syndrome database. After 1 year IFX therapy, intestinal BS patients with non-mucosal healing (NMH, intestinal ulcers detected by colonoscopy) and/or no clinical remission [NCR, scores of the disease activity index for intestinal Behçet's disease (DAIBD) ≥20] were defined as IFX refractory intestinal BS. Multivariate logistic regression analysis was performed to evaluate the predictors for NMH and NCR in IFX refractory intestinal BS. RESULTS: In 85 intestinal BS patients, NMH was identified in 29 (34.12%) patients, and NCR was confirmed in 20 (23.53%) patients. Erythrocyte sedimentation rate (ESR; ≥24 mm/h) and free triiodothyronine (fT3; ≤3.3pmol/L) were the independent risk factors of NMH in IFX refractory intestinal BS. Drinking alcohol and the fT3/free thyroxine ratio (fT3/fT4; ≤0.24) were independent risk factors, and thalidomide was an independent protective factor, for NCR in intestinal BS patients treated by IFX. CONCLUSION: This study may be applicable for adjusting the therapeutic strategy and sidestepping unnecessary exposure to IFX in intestinal BS patients. Routine assessments of ESR, fT3, and fT3/fT4 ratio are helpful to identify high-risk individuals of IFX refractory intestinal BS. Thalidomide is suggested to be a concomitant therapy with IFX for intestinal BS patients.


Assuntos
Síndrome de Behçet , Enteropatias , Humanos , Infliximab , Síndrome de Behçet/diagnóstico , Síndrome de Behçet/tratamento farmacológico , Talidomida/uso terapêutico , Estudos Retrospectivos , Resultado do Tratamento , China , Enteropatias/diagnóstico , Enteropatias/tratamento farmacológico , Enteropatias/induzido quimicamente
13.
J Am Chem Soc ; 144(4): 1700-1708, 2022 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-35041406

RESUMO

The benefits of excess PbI2 on perovskite crystal nucleation and growth are countered by the photoinstability of interfacial PbI2 in perovskite solar cells (PSCs). Here we report a simple chemical polishing strategy to rip PbI2 crystals off the perovskite surface to decouple these two opposing effects. The chemical polishing results in a favorable perovskite surface exhibiting enhanced luminescence, prolonged carrier lifetimes, suppressed ion migration, and better energy level alignment. These desired benefits translate into increased photovoltages and fill factors, leading to high-performance mesostructured formamidinium lead iodide-based PSCs with a champion efficiency of 24.50%. As the interfacial ion migration paths and photodegradation triggers, dominated by PbI2 crystals, were eliminated, the hysteresis of the PSCs was suppressed and the device stability under illumination or humidity stress was significantly improved. Moreover, this new surface polishing strategy can be universally applicable to other typical perovskite compositions.

14.
Cancer ; 128(7): 1402-1410, 2022 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-35077579

RESUMO

BACKGROUND: The correlation between intestinal microbiota and clinical outcomes after allogeneic hematopoietic stem cell transplantation (allo-HCT) has been reported in platforms with T-cell depletion or postcyclophosphamide-based graft-vs-host disease (GVHD) prophylaxis regimens. It is still unclear whether it is the same in platforms of antithymocyte globulin (ATG)-based myeloablative allo-HCT. METHODS: A total of 603 fecal specimens from 100 consecutive patients receiving allo-HCT were collected between December 2018 and July 2020. Fetal samples were profiled with next-generation sequencing of bacterial 16S ribosomal RNA (rRNA) genes. RESULTS: The diversity decreased to the lowest level at approximately day 12 after allo-HCT and then increased over time. According to the diversity of 314 samples that were collected from 86 patients during the engraftment period, patients were grouped into the low- and high-diversity groups. Two-year overall survival in the high-diversity group was significantly longer than that in the low-diversity group (83.7% vs 60.6%, P = .026). Further analysis revealed that worse outcomes for patients with low diversity were associated with increased risk of worse outcomes for patients with low diversity (adjusted hazard ratio, 4.95; P = .046). Its association with relapse and GVHD was not found. Compositional analysis of fecal microbiota revealed that the abundance of bacteroides decreased greatly during allo-HCT, whereas that of Enterococcus, Klebsiella, and Escherichia was found to be increased. CONCLUSIONS: This study indicates that gut dysbiosis in platforms of ATG-based myeloablative allo-HCT featured loss of bacterial diversity. The diversity of the intestinal flora at the engraftment period was an independent predictor of longer survival. LAY SUMMARY: The correlation between intestinal microbiota and clinical outcomes after allogeneic hematopoietic stem cell transplantation (allo-HCT) is reported in platforms with T-cell depletion or postcyclophosphamide-based graft-vs-host disease (GVHD) prophylaxis regimens. It is still unclear whether it is the same pattern in platforms of antithymocyte globulin (ATG)-based T-cell repletion myeloablative allo-HCT. Our study indicated that gut dysbiosis in platforms of ATG-based myeloablative allo-HCT also features loss of bacterial diversity. The diversity of the intestinal flora at the engraftment period is an independent predictor of longer survival.


Assuntos
Microbioma Gastrointestinal , Doença Enxerto-Hospedeiro , Transplante de Células-Tronco Hematopoéticas , Soro Antilinfocitário/uso terapêutico , Doença Enxerto-Hospedeiro/etiologia , Doença Enxerto-Hospedeiro/prevenção & controle , Transplante de Células-Tronco Hematopoéticas/efeitos adversos , Humanos , Condicionamento Pré-Transplante/efeitos adversos , Transplante Homólogo/efeitos adversos
15.
Small ; 18(8): e2105825, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34889023

RESUMO

Organic electrode materials with the advantages of renewability, environment-friendliness, low cost, and high capacity have received widespread attention in recent years for sodium-ion batteries. However, small molecular organic materials suffer from issues such as low conductivity and the high dissolution rate in electrolytes. Herein, a phthalocyanine derivative (TPcDS) with a large non-localized π-electron system, obtained through thermodynamic polymerization of 4-aminophthalonitrile (AP) monomers, is designed to address these issues. According to the density function theory calculation, six sodium ions can be attracted by one polymer molecule, indicating a high theoretical capacity of 375 mA h g-1 . The TPcDS molecule realizes sodium storage through a non-localized π-electron system of phthalocyanine macrocycles. When employed as an anode material for sodium-ion batteries, the functional groups of phthalocyanine macrocycles, such as CN groups in TPcDS, experience obviously reversible structural variation upon discharge/charge. A high reversible capacity of 364 mAh g-1 is achieved at a current density of 0.05 A g-1 , and a charge capacity of as high as 246 mAh g-1 is still maintained after 500 cycles at 0.1 A g-1 . This work provides an effective strategy for the design and synthesis of new oligomeric organic electrode materials.

16.
Small ; 18(23): e2107834, 2022 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-35532078

RESUMO

As the power conversion efficiency (PCE) of organic photovoltaics (OPVs) approaches 19%, increasing research attention is being paid to enhancing the device's long-term stability. In this study, a robust interface engineering of graphene oxide nanosheets (GNS) is expounded on improving the thermal and photostability of non-fullerene bulk-heterojunction (NFA BHJ) OPVs to a practical level. Three distinct GNSs (GNS, N-doped GNS (N-GNS), and N,S-doped GNS (NS-GNS)) synthesized through a pyrolysis method are applied as the ZnO modifier in inverted OPVs. The results reveal that the GNS modification introduces passivation and dipole effects to enable better energy-level alignment and to facilitate charge transfer across the ZnO/BHJ interface. Besides, it optimizes the BHJ morphology of the photoactive layer, and the N,S doping of GNS further enhances the interaction with the photoactive components to enable a more idea BHJ morphology. Consequently, the NS-GNS device delivers enhanced performance from 14.5% (control device) to 16.5%. Moreover, the thermally/chemically stable GNS is shown to stabilize the morphology of the ZnO electron transport layer (ETL) and to endow the BHJ morphology of the photoactive layer grown atop with a more stable thermodynamic property. This largely reduces the microstructure changes and the associated charge recombination in the BHJ layer under constant thermal/light stresses. Finally, the NS-GNS device is demonstrated to exhibit an impressive T80 lifetime (time at which PCE of the device decays to 80% of the initial PCE) of 2712 h under a constant thermal condition at 65 °C in a glovebox and an outstanding photostability with a T80 lifetime of 2000 h under constant AM1.5G 1-sun illumination in an N2 -controlled environment.

17.
Opt Express ; 30(8): 12228-12236, 2022 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-35472862

RESUMO

Bragg grating (BG) filters play important roles in integrated photonics such as signal processing and optical sensing. In silicon-based counterpart photonic platforms, the application of narrow-bandwidth (Δλ) filters is often restrained by fabrication limitations. In this study, narrow-bandwidth BG filters based on Ge-Sb-Se chalcogenide materials are investigated. The structure of the filter is designed by optimizing the grating period, corrugation height, and grating number. The large corrugation of chalcogenide BG is more friendly and convenient for manufacturing process. The symmetric and asymmetric corrugation filters are then fabricated and characterized. Experimental results show a half-maximum bandwidth of 0.97 nm and 0.32 nm for symmetric and asymmetric filters, respectively, which demonstrates excellent narrow-bandwidth filtering performance of chalcogenide BG.

18.
J Org Chem ; 87(18): 12477-12481, 2022 09 16.
Artigo em Inglês | MEDLINE | ID: mdl-36070608

RESUMO

Given the importance of both the CF3 group and the alkyne moiety in synthetic/medicinal chemistry, we report here the first example of efficient synthesis of 2-pyrazolines with a CF3- and alkyne-substituted quaternary carbon center. This methodology has the advantages of high functional group compatibility, the avoidance of base and open-flask conditions, easily available and easy to handle reagent, and broad substrate scope. Notably, this protocol allows for the late-stage functionalization of biologically active molecules and the gram-scale synthesis.


Assuntos
Alcinos , Carbono , Alcinos/química , Ciclização , Reação de Cicloadição , Estrutura Molecular
19.
Clin Exp Rheumatol ; 40(8): 1480-1490, 2022 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34665700

RESUMO

OBJECTIVES: MicroRNAs (miRNAs) derived from plasma exosomes are potential diagnostic biomarkers. However, little is known about the expression of miRNAs derived from plasma exosomes in patients with intestinal Behçet's syndrome (BS). This study aimed to explore the difference of miRNAs derived from plasma exosomes between intestinal BS patients and healthy people, and further identify potential biomarkers that predict the disease activity of intestinal BS. METHODS: A total of 43 intestinal BS patients and 23 healthy volunteers were enrolled, among whom 23 were active intestinal BS and 20 were stable intestinal BS. The miRNAs expression profiles of plasma exosomes in 3 active intestinal BS patients and 3 healthy volunteers were determined using next-generation high throughput sequencing. Additionally, significantly differentially expressed miRNAs were further analysed by quantitative real-time polymerase chain reaction (qRT-PCR) in a validation cohort of 60 subjects. RESULTS: From the sequencing analysis, 15 miRNAs were identified to be differently expressed (p<0.05). Of these, 13 miRNAs were up-regulated, and 2 were down-regulated in intestinal BS patients compared with healthy volunteers. Furthermore, qRT-PCR analysis confirmed that miR-141-3p was down-regulated and miR-122-5p, miR-150-3p, miR-183-5p, miR-224-5p and miR-342-5p were up-regulated in intestinal BS patients' plasma exosomes. Additionally, the level of miR-141-3p was negatively correlated with disease activity indicators of intestinal BS, while miR-122-5p, miR-150-3p, miR-183-5p, miR-224-5p and miR-342-5p was positively correlated with disease activity indicators of intestinal BS. CONCLUSIONS: Circulating miR-141-3p, miR-122-5p, miR-150-3p, miR-183-5p, miR-224-5p and miR-342-5p derived from plasma exosomes may serve as biomarkers of disease activity in intestinal BS.


Assuntos
Síndrome de Behçet , Exossomos , MicroRNAs , Síndrome de Behçet/diagnóstico , Síndrome de Behçet/genética , Síndrome de Behçet/metabolismo , Biomarcadores Tumorais , Exossomos/genética , Exossomos/metabolismo , Perfilação da Expressão Gênica , Humanos , MicroRNAs/metabolismo
20.
Inorg Chem ; 61(30): 12023-12032, 2022 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-35839144

RESUMO

Robust oxygen reduction electrocatalysis is central to renewable fuel cells and metal-air batteries. Herein, Pt nanoparticles (NPs) rooted on porous molybdenum nitride microrods (Pt/Mo2N MRs) are rationally constructed toward the oxygen reduction reaction (ORR). Owing to the desired composition with strong electronic metal-support interactions (EMSIs) and a porous one-dimensional structure supporting ultrafine NPs, the developed Pt/Mo2N MRs possess much higher ORR mass and specific activities than commercial Pt/C. In situ Raman and density functional theory calculations reveal that the EMSI weakens the adsorption of intermediates over Pt/Mo2N MRs via an associative mechanism. Moreover, the porous Mo2N support stabilizes these high activities. Impressively, a homemade zinc-air battery driven by Pt/Mo2N MRs delivers excellent performance including a peak power density of 167 mW cm-2 and a high rate capability that ranged from 5 to 50 mA cm-2. This work highlights the role of EMSI in promoting robust ORR electrocatalysis, thus providing a promising approach for efficient and robust cathode materials for advanced metal-air batteries.

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