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1.
Angew Chem Int Ed Engl ; : e202404713, 2024 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-38670925

RESUMO

Methanol oxidation plays a central role to implement sustainable energy economy, which is restricted by the sluggish reaction kinetics due to the multi-electron transfer process accompanied by numerous sequential intermediate. In this study, an efficient cascade methanol oxidation reaction is catalyzed by single-Ir-atom catalyst at ultra-low potential (< 0.1 V) with the promotion of the thermal and electrochemical integration in a high temperature polymer electrolyte membrane electrolyzer. At the elevated temperature, the electron deficient Ir site with higher methanol affinity could spontaneous catalyze the CH3OH dehydrogenation to CO under the voltage, then the generated CO and H2 was electrochemically oxidized to CO2 and proton. However, the methanol cannot thermally decompose with the voltage absence, which confirm the indispensable of the coupling of thermal and electrochemical integration for the methanol oxidation. By assembling the methanol oxidation reaction with hydrogen evolution reaction in the HT-PEME with single-Ir-atom catalysts in the anode chamber, a max hydrogen production rate reaches 18 mol gIr-1 h-1, which is much greater than that of Ir nanoparticles and commercial Pt/C catalyst. This study also demonstrated the electrochemical MOR activity of the single atom catalysts, which broadens the renewable energy devices and the catalyst design by an integration concept.

2.
Angew Chem Int Ed Engl ; 63(7): e202315157, 2024 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-38143245

RESUMO

Methanol steam reforming (MSR) provides an alternative way for efficient production and safe transportation of hydrogen but requires harsh conditions and complicated purification processes. In this work, an efficient electrochemical-assisted MSR reaction for pure H2 production at lower temperature (~140 °C) is developed by coupling the electrocatalysis reaction into the MSR in a polymer electrolyte membrane electrolysis reactor. By electrochemically assisted, the two critical steps including the methanol dehydrogenation and water-gas shift reaction are accelerated, which is attributed to decreasing the methanol dehydrogenation energy and promoting the dissociation of H2 O to OH* by the applied potential. Furthermore, the reduced H2 partial pressure by the hydrogen oxidation and reduction process further promotes MSR. The combination of these advantages not only efficiently decreases the MSR temperature but also achieves the high rate of hydrogen production of 505 mmol H2 g Pt -1 h-1 with exceptionally high H2 selectivity (99 %) at 180 °C and a low voltage (0.4 V), and the productivity is about 30-fold than that of traditional MSR. This study opens up a new avenue to design novel electrolysis cells for hydrogen production.

3.
Sci Rep ; 13(1): 11011, 2023 07 07.
Artigo em Inglês | MEDLINE | ID: mdl-37419935

RESUMO

Marine microplastics are emerging as a growing environmental concern due to their potential harm to marine biota. The substantial variations in their physical and chemical properties pose a significant challenge when it comes to sampling and characterizing small-sized microplastics. In this study, we introduce a novel microfluidic approach that simplifies the trapping and identification process of microplastics in surface seawater, eliminating the need for labeling. We examine various models, including support vector machine, random forest, convolutional neural network (CNN), and residual neural network (ResNet34), to assess their performance in identifying 11 common plastics. Our findings reveal that the CNN method outperforms the other models, achieving an impressive accuracy of 93% and a mean area under the curve of 98 ± 0.02%. Furthermore, we demonstrate that miniaturized devices can effectively trap and identify microplastics smaller than 50 µm. Overall, this proposed approach facilitates efficient sampling and identification of small-sized microplastics, potentially contributing to crucial long-term monitoring and treatment efforts.


Assuntos
Técnicas Analíticas Microfluídicas , Água do Mar , Técnicas Analíticas Microfluídicas/instrumentação , Técnicas Analíticas Microfluídicas/métodos , Água do Mar/química , Plásticos/química , Aprendizado de Máquina , Poluentes Químicos da Água/química
4.
Biosens Bioelectron ; 236: 115426, 2023 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-37276636

RESUMO

Microfluidic technology has emerged as a promising tool in various applications, including biosensing, disease diagnosis, and environmental monitoring. One of the notable features of microfluidic devices is their ability to selectively capture and release specific cells, biomolecules, bacteria, and particles. Compared to traditional bulk analysis instruments, microfluidic capture-and-release platforms offer several advantages, such as contactless operation, label-free detection, high accuracy, good sensitivity, and minimal reagent requirements. However, despite significant efforts dedicated to developing innovative capture mechanisms in the past, the release and recovery efficiency of trapped particles have often been overlooked. Many previous studies have focused primarily on particle capture techniques and their efficiency, disregarding the crucial role of successful particle release for subsequent analysis. In reality, the ability to effectively release trapped particles is particularly essential to ensure ongoing, high-throughput analysis. To address this gap, this review aims to highlight the importance of both capture and release mechanisms in microfluidic systems and assess their effectiveness. The methods are classified into two categories: those based on physical principles and those using biochemical approaches. Furthermore, the review offers a comprehensive summary of recent applications of microfluidic platforms specifically designed for particle capture and release. It outlines the designs and performance of these devices, highlighting their advantages and limitations in various target applications and purposes. Finally, the review concludes with discussions on the current challenges faced in the field and presents potential future directions.


Assuntos
Técnicas Biossensoriais , Técnicas Analíticas Microfluídicas , Microfluídica/métodos , Dispositivos Lab-On-A-Chip , Monitoramento Ambiental
5.
G3 (Bethesda) ; 13(6)2023 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-37154439

RESUMO

Maintaining a definite and stable pool of dividing stem cells plays an important role in organ development. This process requires an appropriate progression of mitosis for proper spindle orientation and polarity to ensure the ability of stem cells to proliferate and differentiate correctly. Polo-like kinases (Plks)/Polo are the highly conserved serine/threonine kinases involved in the initiation of mitosis as well as in the progression of the cell cycle. Although numerous studies have investigated the mitotic defects upon loss of Plks/Polo in cells, little is known about the in vivo consequences of stem cells with abnormal Polo activity in the context of tissue and organism development. The current study aimed to investigate this question using the Drosophila intestine, an organ dynamically maintained by the intestinal stem cells (ISCs). The results indicated that the polo depletion caused a reduction in the gut size due to a gradual decrease in the number of functional ISCs. Interestingly, the polo-deficient ISCs showed an extended G2/M phase and aneuploidy and were subsequently eliminated by premature differentiation into enterocytes (ECs). In contrast, the constitutively active Polo (poloT182D) suppressed ISC proliferation, induced abnormal accumulation of ß-tubulin in cells, and drove ISC loss via apoptosis. Therefore, Polo activity should be properly maintained for optimal stem cell function. Further analysis suggested that polo was a direct target gene of Sox21a, a Sox transcription factor that critically regulates stem cell activity. Together, this study provided a novel perspective on the correlation between the progression of mitosis and the ISC function in Drosophila.


Assuntos
Proteínas de Drosophila , Drosophila , Animais , Ciclo Celular/genética , Proteínas de Ciclo Celular/genética , Proteínas de Ciclo Celular/metabolismo , Drosophila/genética , Drosophila/metabolismo , Proteínas de Drosophila/metabolismo , Intestinos , Mitose/genética , Células-Tronco/metabolismo
6.
Micromachines (Basel) ; 13(4)2022 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-35457804

RESUMO

Plastic pollution has emerged as a growing concern worldwide. In particular, the most abundant plastic debris, microplastics, has necessitated the development of rapid and effective identification methods to track down the stages and evidence of the pollution. In this paper, we combine low-cost plastic staining technologies using Nile Red with the continuous feature offered by microfluidics to propose a low-cost 3D printed device for the identification of microplastics. It is observed that the microfluidic devices indicate comparable staining and identification performance compared to conventional Nile Red staining processes while offering the advantages of continuous recognition for long-term environmental monitoring. The results also show that concentration, temperature, and residency time possess strong effects on the identification performance. Finally, various microplastics have been applied to further demonstrate the effectiveness of the proposed devices. It is found that, among different types of microplastics, non-spherical microplastics show the maximal fluorescence level. Meanwhile, natural fibers indicate better staining quality when compared to synthetic ones.

7.
Dev Comp Immunol ; 131: 104361, 2022 06.
Artigo em Inglês | MEDLINE | ID: mdl-35143809

RESUMO

Prophenoloxidase (PPO), an important immunity protein in insects, is mainly produced by hemocytes and released into the hemolymph upon cell lysis. In addition, PPO can also be produced by epidermal cells in the foregut to detoxify the toxic plant secondary metabolites and in the hindgut to kill pathogens through PPO-induced melanization. Previously, we noticed a pair of tubes extended from the larval hindgut became melanized upon staining in dopamine dissolved in 30% ethanol. However, the structure and function of these tubes are largely unknown. In this study, we performed staining of the tubes and the neighboring Malpighian tubule for further confirmation. Eventually, we detected PPO inside epidermal cells of the tubes, and called them as PPO-positive tubes. We observed that the PPO-positive tubes are physically derived from the hindgut but strongly adhere to the Malpighian tubule. Inside the PPO-positive tubes, there is an acellular peritrophic membrane to protect the epidermal cells. Furthermore, the PPO-positive tubes act like a doorkeeper to firstly detoxify the metabolite wastes collected by the Malpighian tubule from the hemolymph.


Assuntos
Lepidópteros , Túbulos de Malpighi , Animais , Catecol Oxidase/metabolismo , Precursores Enzimáticos/metabolismo , Túbulos de Malpighi/metabolismo
8.
Front Immunol ; 12: 741797, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34603328

RESUMO

Entomopathogenic fungi Beauveria bassiana can infect many species of insects and is used as a biological pesticide world-wide. Before reaching the hemocoel, B. bassiana has to penetrate the integument which is composed of a thick chitin layer and epidermal cells. Some chitinase, protease and lipase secreted by B. bassiana are probably involved in the fungal penetration of the integument. While microscopic proof is needed, it is difficult to locate the precise infection sites following the traditional method of immersion infection. Consequently, we developed a new method to inoculate conidia solution into a single fixed-site on the back of one segment. This fixed-site infection method is pathogenic but it is also dose dependent. Using the fixed-site infection protocol, it is also very convenient to track hyphae inside the cuticle layer by light and transmission electron microscopy. The fact that few hyphae were detected inside the chitin layer after fixed-site infection with mutant ΔBPS8, a protease secreted during fungi germination, indicates that this method is suitable for screening genes involved in penetrating the integument in large scale. We also found that melanization occurs before new hyphae penetrate the chitin layer. Most importantly, we discovered that fungal infection can induce epidermal cell proliferation through DNA duplication and cell division, which is essential for the host to defend against fungal infection. Taken together the fixed-site infection method may be helpful to determine the mechanism of fungal and host interaction in the integument so as to effectively exert fungal biological virulence.


Assuntos
Beauveria/fisiologia , Bombyx/imunologia , Quitina/metabolismo , Epiderme/metabolismo , Micoses/imunologia , Animais , Proliferação de Células , Quitinases/metabolismo , Epiderme/patologia , Interações entre Hospedeiro e Microrganismos , Hifas , Proteínas de Insetos/metabolismo , Lipase/metabolismo , Microscopia Eletrônica de Transmissão , Mutação/genética , Peptídeo Hidrolases/metabolismo , Controle de Pragas , Esporos Fúngicos , Virulência
9.
Angew Chem Int Ed Engl ; 59(33): 13923-13928, 2020 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-32436324

RESUMO

The applications of the most promising Fe-N-C catalysts are prohibited by their limited intrinsic activities. Manipulating the Fe energy level through anchoring electron-withdrawing ligands is found effective in boosting the catalytic performance. However, such regulation remains elusive as the ligands are only uncontrollably introduced oweing to their energetically unstable nature. Herein, we report a rational manipulation strategy for introducing axial bonded O to the Fe sites, attained through hexa-coordinating Fe with oxygen functional groups in the precursor. Moreover, the O modifier is stabilized by forming the Fe-O-Fe bridge bond, with the approximation of two FeN4 sites. The energy level modulation thus created confers the sites with an intrinsic activity that is over 10 times higher than that of the normal FeN4 site. Our finding opens a novel strategy to manage coordination environments at an atomic level for high activity ORR catalysts.

10.
Angew Chem Int Ed Engl ; 58(36): 12469-12475, 2019 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-31290248

RESUMO

Single-atom catalysts (SACs) are attracting widespread interest for the catalytic oxygen reduction reaction (ORR), with Fe-Nx SACs exhibiting the most promising activity. However, Fe-based catalysts suffer serious stability issues as a result of oxidative corrosion through the Fenton reaction. Herein, using a metal-organic framework as an anchoring matrix, we for the first time obtained pyrolyzed Cr/N/C SACs for the ORR, where the atomically dispersed Cr is confirmed to have a Cr-N4 coordination structure. The Cr/N/C catalyst exhibits excellent ORR activity with an optimal half-wave potential of 0.773 V versus RHE. More excitingly, the Fenton reaction is substantially reduced and, thus, the final catalysts show superb stability. The innovative and robust active site for the ORR opens a new possibility to circumvent the stability issue of the non-noble metal ORR catalysts.

11.
Res Dev Disabil ; 79: 130-141, 2018 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-29422422

RESUMO

BACKGROUND: Despite positive effects of and established empirical evidence for tablet-based interventions for individuals with autism spectrum disorder (ASD), it is not known whether such findings can be applicable to maintenance and generalization effects of those interventions. AIMS: This systematic review evaluated peer-reviewed single-case experimental design (SCED) studies concerning evidence of generalization and maintenance effects of tablet-based interventions for individuals with ASD. METHODS: To evaluate the methodological rigor of the literature in terms of generalization and maintenance effects, the authors adopted four of the basic design standards developed by What Works Clearinghouse (WWC; Kratochwill et al., 2010/2014). In addition, the authors used Tau-U effect size measure and attempted to calculate effect sizes differentiated by the type of generalization and maintenance teaching strategies. RESULTS: A total of 21 studies assessed generalization and/or maintenance effects. In the first evaluation of evidence of generalization and maintenance effects, it was found that more than half of the studies included in this review collected interobserver agreement (IOA) on at least 20% of sessions across all generalization and maintenance conditions and met the minimum quality thresholds of IOA. Meanwhile, less than one third of the studies included more than three data points in each generalization and maintenance condition. With regard to maintenance of effects, about half of the reviewed studies did not report the latency to the maintenance measure, which may hamper the assessment of the clinical and practical significance of the effect of the tablet-based intervention. In the second evaluation, the omnibus Tau-U effect size for baseline to generalization comparisons resulted in a moderate effect. For the contrasts between intervention and generalization comparisons resulted in a small effect. The omnibus Tau-U effect size for baseline and maintenance comparisons resulted in a strong effect. For the contrasts between intervention to maintenance comparisons, the omnibus Tau-U effect size resulted in a small effect. CONCLUSIONS AND IMPLICATION: Findings in this review suggest that efforts should be made to establish a system for appraising generalization and maintenance procedures in SCED studies. In addition, future studies should investigate if tablet-based interventions are truly effective in creating sustainable behavioral change in individuals with ASD.


Assuntos
Sintomas Comportamentais/terapia , Computadores de Mão , Educação Inclusiva/métodos , Transtorno do Espectro Autista , Confiabilidade dos Dados , Humanos , Administração dos Cuidados ao Paciente/métodos
12.
Res Dev Disabil ; 70: 198-214, 2017 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-28964654

RESUMO

BACKGROUND: There is a growing amount of single-case research literature on the benefits of tablet-mediated interventions for individuals with autism spectrum disorder (ASD). With the development of tablet-based computers, tablet-mediated interventions have been widely utilized for education and treatment purposes; however, the overall quality and evidence of this literature-base are unknown. AIMS: This article aims to present a quality review of the single-case experimental literature and aggregate results across studies involving the use of tablet-mediated interventions for individuals with ASD. METHODS AND PROCEDURES: Using the Tau nonoverlap effect size measure, the authors extracted data from single-case experimental studies and calculated effect sizes differentiated by moderator variables. The moderator variables included the ages of participants, participants' diagnoses, interventions, outcome measures, settings, and contexts. OUTCOMES AND RESULTS: Results indicate that tablet-mediated interventions for individuals with ASD have moderate to large effect sizes across the variables evaluated. The majority of research in this review used tablets for video modeling and augmentative and alternative communication. CONCLUSIONS AND IMPLICATIONS: To promote the usability of tablet-mediated interventions for individuals with ASD, this review indicates that more single-case experimental studies should be conducted with this population in naturalistic home, community, and employment settings.


Assuntos
Transtorno do Espectro Autista/reabilitação , Computadores de Mão , Desempenho Acadêmico , Atividades Cotidianas , Auxiliares de Comunicação para Pessoas com Deficiência , Sinais (Psicologia) , Emprego , Humanos , Aplicativos Móveis , Habilidades Sociais
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