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1.
Chem Rec ; 24(1): e202300183, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37642262

RESUMO

Perovskite solar cells (PSCs) have rapidly become a prevalent photovoltaic technology owing to their simple structure, low processing cost, and remarkable increase in solar-to-electric power conversion efficiency (PCE). However, the intermittent nature of solar radiation induces some technical and financial challenges for its practical applications as a reliable power source. To address this issue, the integration of PSCs with supercapacitors (SCs) in the form of integrated photo-supercapacitors (IPSs) has gathered significant attention. This integration can balance energy availability and demand, reduce energy wastage, and stabilize power output for portable and wearable electronics. Meanwhile, the excellent optoelectronic properties with mixed electronic and ionic conductivity of metal halide perovskites (MHPs) have expanded their application as electrode and electrolyte materials for SCs and photo-supercapacitors (PSs) applications. This review provides an all-inclusive summary of the current state-of-the-art research progress of PSCs-IPSs and MHPs-based SCs and PSs by highlighting their basics and integration approaches. It also discusses the challenges and prospects of these materials and technologies.

2.
Sensors (Basel) ; 24(7)2024 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-38610384

RESUMO

With the wide applications of the Internet of Things (IoT) in smart home systems, IEEE 802.11n Wireless Local Area Networks (WLANs) have become a frequently chosen communication technology due to their adaptability and affordability. In a high-density network of devices such as the smart home scenerio, a host often meets interferences from other devices and unequal Received Signal Strength (RSS) from Access Points (APs). This results in throughput unfairness/insufficiency problems between hosts communicating concurrently in WLAN. Previously, we have studied the throughput request satisfaction method to address this problem. It calculates the target throughput from measured single and concurrent throughputs of hosts and controls the actual throughput at this target one by applying traffic shaping at the AP. However, the insufficiency problem of maximizing the throughput is not solved due to interferences from other hosts. In this paper, we present an extension of the throughput request satisfaction method to maximize the throughput of a high-priority host under concurrent communications. It recalculates the target throughput to increase the actual throughput as much as possible while the other hosts satisfy the least throughput. For evaluations, we conduct experiments using the test-bed system with Raspberry Pi as the AP devices in several topologies in indoor environments. The results confirm the effectiveness of our proposal.

3.
J Org Chem ; 88(19): 13371-13391, 2023 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-36054817

RESUMO

Ground-state destabilization of the N-C(O) linkage represents a powerful tool to functionalize the historically inert amide bond. This burgeoning reaction manifold relies on the availability of amide bond precursors that participate in weakening of the nN → π*C=O conjugation through N-C twisting, N pyramidalization, and nN electronic delocalization. Since 2015, acyl N-C amide bond activation through ground-state destabilization of the amide bond has been achieved by transition-metal-catalyzed oxidative addition of the N-C(O) bond, generation of acyl radicals, and transition-metal-free acyl addition. This Perspective summarizes contributions of our laboratory in the development of new ground-state-destabilized amide precursors enabled by twist and electronic activation of the amide bond and synthetic utility of ground-state-destabilized amides in cross-coupling reactions and acyl addition reactions. The use of ground-state-destabilized amides as electrophiles enables a plethora of previously unknown transformations of the amide bond, such as acyl coupling, decarbonylative coupling, radical coupling, and transition-metal-free coupling to forge new C-C, C-N, C-O, C-S, C-P, and C-B bonds. Structural studies of activated amides and catalytic systems developed in the past decade enable the view of the amide bond to change from the "traditionally inert" to "readily modifiable" functional group with a continuum of reactivity dictated by ground-state destabilization.

4.
Int J Equity Health ; 22(1): 111, 2023 06 06.
Artigo em Inglês | MEDLINE | ID: mdl-37277825

RESUMO

BACKGROUND: Infection Prevention and Control (IPC) is critical in controlling the COVID-19 pandemic and is one of the pillars of the WHO COVID-19 Strategic Preparedness and Response Plan 2020. We conducted an Intra-Action Review (IAR) of IPC response efforts to the COVID-19 pandemic in Cox's Bazar, Bangladesh, to identify best practices, challenges, and recommendations for improvement of the current and future responses. METHODS: We conducted two meetings with 54 participants purposively selected from different organizations and agencies involved in the frontline implementation of IPC in Cox's Bazar district, Bangladesh. We used the IPC trigger questions from the WHO country COVID-19 IAR: trigger question database to guide the discussions. Meeting notes and transcripts were then analyzed manually using content analysis, and results were presented in text and quotes. RESULTS: Best practices included: assessments, a response plan, a working group, trainings, early case identification and isolation, hand hygiene in Health Facilities (HFs), monitoring and feedback, general masking in HFs, supportive supervision, design, infrastructure and environmental controls in Severe Acute Respiratory Infection Isolation and Treatment Centers (SARI ITCs) and HFs and waste management. Challenges included: frequent breakdown of incinerators, limited PPE supply, inconsistent adherence to IPC, lack of availability of uniforms for health workers, in particular cultural and gender appropriate uniforms and Personal Protective Equipment (PPE). Recommendations from the IAR were: (1) to promote the institutionalization of IPC, programs in HFs (2) establishment of IPC monitoring mechanisms in all HCFs, (3) strengthening IPC education and training in health care facilities, and (4) strengthen public health and social measures in communities. CONCLUSION: Establishing IPC programmes that include monitoring and continuous training are critical in promoting consistent and adaptive IPC practices. Response to a pandemic crisis combined with concurrent emergencies, such as protracted displacement of populations with many diverse actors, can only be successful with highly coordinated planning, leadership, resource mobilization, and close supervision.


Assuntos
COVID-19 , Refugiados , Humanos , COVID-19/prevenção & controle , Bangladesh , Campos de Refugiados , Pandemias/prevenção & controle , Controle de Infecções
5.
Molecules ; 28(15)2023 Aug 02.
Artigo em Inglês | MEDLINE | ID: mdl-37570803

RESUMO

In this Special Issue, "Featured Papers in Organometallic Chemistry", we report on the synthesis and characterization of [IPr#-PEPPSI], a new, well-defined, highly hindered Pd(II)-NHC precatalyst for cross-coupling reactions. This catalyst was commercialized in collaboration with MilliporeSigma, Burlington, ON, Canada (no. 925489) to provide academic and industrial researchers with broad access to reaction screening and optimization. The broad activity of [IPr#-PEPPSI] in cross-coupling reactions in a range of bond activations with C-N, C-O, C-Cl, C-Br, C-S and C-H cleavage is presented. A comprehensive evaluation of the steric and electronic properties is provided. Easy access to the [IPr#-PEPPSI] class of precatalysts based on modular pyridine ligands, together with the steric impact of the IPr# peralkylation framework, will facilitate the implementation of well-defined, air- and moisture-stable Pd(II)-NHC precatalysts in chemistry research.

6.
Chemistry ; 28(4): e202103341, 2022 Jan 19.
Artigo em Inglês | MEDLINE | ID: mdl-34773313

RESUMO

A new class of large-but-flexible Pd-BIAN-NHC catalysts (BIAN=acenaphthoimidazolylidene, NHC=N-heterocyclic carbene) has been rationally designed to enable the challenging Buchwald-Hartwig amination of coordinating heterocycles. This robust class of BIAN-NHC catalysts permits cross-coupling under practical aerobic conditions of a variety of heterocycles with aryl, alkyl, and heteroarylamines, including historically challenging oxazoles and thiazoles as well as electron-deficient heterocycles containing multiple heteroatoms with BIAN-INon (N,N'-bis(2,6-di(4-heptyl)phenyl)-7H-acenaphtho[1,2-d]imidazol-8-ylidene) as the most effective ligand. Studies on the ligand structure and electronic properties of the carbene center are reported. The study should facilitate the discovery of even more active catalyst systems based on the unique BIAN-NHC scaffold.


Assuntos
Compostos Heterocíclicos , Aminação , Catálise , Ligantes , Paládio
7.
Sens Actuators B Chem ; 359: 131591, 2022 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-35221530

RESUMO

This paper reports on an ultrasensitive and label-free electrochemical immunosensor for monitoring the SARS-CoV-2 spike protein (SARS-CoV-2 SP). A self-supported electrode, which can simultaneously serve as an antibody immobilization matrix and electron transport channel, was initially fabricated by a controlled partial exfoliation of a flexible graphitic carbon foil (GCF). Mild acidic treatment enabled the partial oxidation and exfoliation (down to a few layers) of the flexible GCF; this also provided a high percentage of oxygen functionality and an enhanced surface roughness. The substrate electrode was further functionalized with ethylenediamine (EDA) to provide a suitable platform with even a higher surface roughness, for the covalent immobilization of an anti-SARS-CoV-2 antibody. The change in the current response for the [Fe(CN)6]3-/4- redox couple, induced by the binding of SARS-CoV-2 SP to the antibody immobilized on the electrode surface, was used to determine the SARS-CoV-2 SP concentration. The immunosensor thus prepared could detect SARS-CoV-2 SP within 30 min with high reproducibility and specificity over a wide concentration range (0.2-100 ng/mL). Detection limits of 25 pg/mL and 27 pg/mL were found in a phosphate buffer solution (pH 7.4), and diluted blood plasma, respectively. The immunosensor was also employed to detect SARS-CoV-2 SP in artificial human saliva.

8.
Lett Appl Microbiol ; 75(4): 813-823, 2022 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-35575585

RESUMO

The present study aimed to characterize and compare the skin and gut microbial communities of rohu at various post-harvest stages of consumption using quantitative real-time polymerase chain reaction and 16S rRNA-based amplicon sequencing. Real-time PCR amplification detected higher copy numbers for coliform bacteria-Escherichia coli, Salmonella enterica and Shigella spp. in the marketed fish-compared to fresh and frozen samples. The 16S rRNA data revealed higher alpha diversity measurements in the skin of fish from different retail markets of Dhaka city. Beta ordination revealed distinct clustering of bacterial OTUs for the skin and gut samples from three different groups. At the phylum level, Proteobacteria was most abundant in all groups except the Fusobacteria in the control fish gut. Although Aeromonas was found ubiquitous in all types of samples, diverse bacterial genera were identified in the marketed fish samples. Nonetheless, low species richness was observed for the frozen fish. Most of the differentially abundant bacteria in the skin samples of marketed fish are opportunistic human pathogens enriched at different stages of postharvest handling and processing. Therefore, considering the microbial contamination in the aquatic environment in Bangladesh, post-harvest handling should be performed with proper methods and care to minimize bacterial transmission into fish.


Assuntos
Cyprinidae , Microbiota , Animais , Bactérias/genética , Bangladesh , Água Doce , Humanos , RNA Ribossômico 16S/genética
9.
Health Commun ; 37(12): 1503-1509, 2022 11.
Artigo em Inglês | MEDLINE | ID: mdl-35996960

RESUMO

COVID-19 has exacerbated existing health inequalities globally. Guided by the culture-centered approach, this study examined perspectives and experiences of healthcare during two lockdowns in four marginalized contexts in Aotearoa New Zealand. The participants' narratives depicted dissatisfaction with the new modes of healthcare delivery, reporting longer waiting times, a preference for face-to-face delivery, language barriers, and issues with the limitations in support people attending appointments. This resulted in healthcare being delivered in a way that was not in keeping with the localized cultural norms of communication and collective support, further exacerbating existing health inequalities. Our findings suggest that public health interventions in response to COVID-19 within the context of healthcare delivery have the potential to further reify and reproduce exclusions and experiences of marginalization, with cultural marginalization reifying structural marginalization.


Assuntos
COVID-19 , COVID-19/epidemiologia , Controle de Doenças Transmissíveis , Barreiras de Comunicação , Atenção à Saúde , Humanos , Pobreza
10.
Sensors (Basel) ; 22(22)2022 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-36433419

RESUMO

Nowadays, the IEEE 802.11 wireless local area network (WLAN) has been widely used for Internet access services around the world. Then, the unfairness or insufficiency in meeting the throughput request can appear among concurrently communicating hosts with the same access point (AP), which should be solved by sacrificing advantageous hosts. Previously, we studied the fairness control method by adopting packet transmission delay at the AP. However, it suffers from slow convergence and may not satisfy different throughput requests among hosts. In this paper, we propose a throughput request satisfaction method for providing fair or different throughput requests when multiple hosts are concurrently communicating with a single AP. To meet the throughput request, the method (1) measures the single and concurrent throughput for each host, (2) calculates the channel occupying time from them, (3) derives the target throughput to achieve the given throughput request, and (4) controls the traffic by applying traffic shaping at the AP. For evaluations, we implemented the proposal in the WLAN testbed system with one Raspberry Pi AP and up to five hosts, and conducted extensive experiments in five scenarios with different throughput requests. The results confirmed the effectiveness of our proposal.


Assuntos
Redes Locais , Satisfação Pessoal , Tecnologia sem Fio
11.
Int J Mol Sci ; 23(24)2022 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-36555495

RESUMO

Diosgenin is a botanical steroidal saponin with immunomodulatory, anti-inflammatory, anti-oxidative, anti-thrombotic, anti-apoptotic, anti-depressant, and anti-nociceptive effects. However, the effects of diosgenin on anti-nociception are unclear. Transient receptor potential vanilloid 1 (TRPV1) plays an important role in nociception. Therefore, we investigated whether TRPV1 antagonism mediates the anti-nociceptive effects of diosgenin. In vivo mouse experiments were performed to examine nociception-related behavior, while in vitro experiments were performed to examine calcium currents in dorsal root ganglion (DRG) and Chinese hamster ovary (CHO) cells. The duration of capsaicin-induced licking (pain behavior) was significantly reduced following oral and intraplantar administration of diosgenin, approaching levels observed in mice treated with the TRPV1 antagonist N-(4-tertiarybutylphenyl)-4-(3-cholorphyridin-2-yl) tetrahydropyrazine-1(2H)-carbox-amide. Additionally, oral administration of diosgenin blocked capsaicin-induced thermal hyperalgesia. Further, diosgenin reduced capsaicin-induced Ca2+ currents in a dose-dependent manner in both DRG and CHO cells. Oral administration of diosgenin also improved thermal and mechanical hyperalgesia in the sciatic nerve constriction injury-induced chronic pain model by reducing the expression of TRPV1 and inflammatory cytokines in DRG cells. Collectively, our results suggest that diosgenin exerts analgesic effects via antagonism of TRPV1 and suppression of inflammation in the DRG in a mouse model of neuropathic pain.


Assuntos
Analgésicos , Diosgenina , Neuralgia , Canais de Cátion TRPV , Animais , Cricetinae , Camundongos , Analgésicos/farmacologia , Capsaicina/farmacologia , Células CHO , Cricetulus , Diosgenina/farmacologia , Modelos Animais de Doenças , Gânglios Espinais/metabolismo , Hiperalgesia/metabolismo , Neuralgia/tratamento farmacológico , Neuralgia/metabolismo , Canais de Cátion TRPV/antagonistas & inibidores , Canais de Cátion TRPV/metabolismo
12.
J Org Chem ; 86(15): 10455-10466, 2021 08 06.
Artigo em Inglês | MEDLINE | ID: mdl-34275281

RESUMO

The development of efficient methods for facilitating N-C(O) bond activation in amides is an important objective in organic synthesis that permits the manipulation of the traditionally unreactive amide bonds. Herein, we report a comparative evaluation of a series of cyclic amides as activating groups in amide N-C(O) bond cross-coupling. Evaluation of N-acyl-imides, N-acyl-lactams, and N-acyl-oxazolidinones bearing five- and six-membered rings using Pd(II)-NHC and Pd-phosphine systems reveals the relative reactivity order of N-activating groups in Suzuki-Miyaura cross-coupling. The reactivity of activated phenolic esters and thioesters is evaluated for comparison in O-C(O) and S-C(O) cross-coupling under the same reaction conditions. Most notably, the study reveals N-acyl-δ-valerolactams as a highly effective class of mono-N-acyl-activated amide precursors in cross-coupling. The X-ray structure of the model N-acyl-δ-valerolactam is characterized by an additive Winkler-Dunitz distortion parameter Σ(τ+χN) of 54.0°, placing this amide in a medium distortion range of twisted amides. Computational studies provide insight into the structural and energetic parameters of the amide bond, including amidic resonance, N/O-protonation aptitude, and the rotational barrier around the N-C(O) axis. This class of N-acyl-lactams will be a valuable addition to the growing portfolio of amide electrophiles for cross-coupling reactions by acyl-metal intermediates.


Assuntos
Amidas , Lactamas , Reações Cruzadas , Imidas , Piperidonas
13.
J Fish Dis ; 44(5): 591-599, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33210340

RESUMO

Vibriosis caused by luminous Vibrio species is one of the biggest challenges to shrimp industry in Bangladesh. This study aimed to characterize whole microbial communities from Vibrio-infected black tiger shrimp (Penaeus monodon) using 16S rRNA-based amplicon sequencing. A total of 36 disease-free and infected shrimp were collected from six different hatcheries in Bagerhat, Bangladesh. A final pool of 12 samples (n = 6) was created by homogenization of the hepatopancreas samples from three shrimps collected from each hatchery for the same group. The amplicon sequencing data revealed significant (p < .05) decrease of alpha diversity measurements and subsequent effects (p < .05) on the hepatopancreas microbiota in the infected group, compared to control shrimp. Proteobateria and Aeromonas were the most dominant bacteria at phylum and genus level in both groups and identified as core microbiota in the community. Two bacterial groups at phyla level and eight at genus level were found associated with the alteration of hepatopancreas microbial communities and associated gene functions in vibriosis-infected shrimp, revealed by differential abundance and KEGG pathway analysis. The overwhelming abundance of Citroibacter, Shewanella and Candidatus lineages in vibriosis-infected shrimp needs further investigations.


Assuntos
Genes Bacterianos , Penaeidae/microbiologia , RNA Bacteriano/genética , RNA Ribossômico 16S/genética , Vibrio/genética , Animais , RNA Bacteriano/metabolismo , RNA Ribossômico 16S/metabolismo , Análise de Sequência de RNA , Vibrio/metabolismo
14.
Mikrochim Acta ; 188(3): 77, 2021 02 10.
Artigo em Inglês | MEDLINE | ID: mdl-33566156

RESUMO

The synthesis of Co-based two-dimensional (2D) metal azolate framework nanosheets (MAF-5-CoII NS) is described using a simple hydrothermal method. The product was isostructural to MAF-5 (Zn). The as-prepared MAF-5-CoII NS exhibited high surface area (1155 m2/g), purity, and crystallinity. The MAF-5-CoII NS-modified screen-printed electrode (MAF-5-CoII NS/SPE) was used for nonenzymatic detection of glucose in diluted human blood plasma (BP) samples with phosphate buffer saline (PBS, pH 7.4) and NaOH (0.1 M, pH 13.0) solutions. The MAF-5-CoII NS nanozyme displayed good redox activity in both neutral and alkaline media with the formation of CoII/CoIII redox pair, which induced the catalytic oxidation of glucose. Under the optimized detection potential, the sensor presented a chronoamperometric current response for the oxidation of glucose with two wide concentration ranges in PBS-diluted (62.80 to 180 µM and 305 to 8055 µM) and NaOH-diluted (58.90 to 117.6 µM and 180 to 10,055 µM) BP samples, which were within the limit of blood glucose levels of diabetic patients before (4.4-7.2 mM) and after (10 mM) meals (recommended by the American Diabetes Association). The sensor has a limit of detection of ca. 0.25 and 0.05 µM, respectively, and maximum sensitivity of ca. 36.55 and 1361.65 mA/cm2/mM, respectively, in PBS- and NaOH-diluted BP samples. The sensor also displayed excellent stability in the neutral and alkaline media due to the existence of hydrophobic linkers (2-ethyl imidazole) in the MAF-5-CoII NS, good repeatability and reproducibility, and interference-free signals. Thus, MAF-5-CoII NS is a promising nanozyme for the development of the disposable type of sensor for glucose detection in human body fluids. Graphical abstract.


Assuntos
Glicemia/análise , Estruturas Metalorgânicas/química , Nanoestruturas/química , Glicemia/química , Catálise , Cobalto/química , Técnicas Eletroquímicas/instrumentação , Técnicas Eletroquímicas/métodos , Eletrodos , Humanos , Concentração de Íons de Hidrogênio , Limite de Detecção , Estruturas Metalorgânicas/síntese química , Oxirredução , Reprodutibilidade dos Testes
15.
Int J Mol Sci ; 22(22)2021 Nov 09.
Artigo em Inglês | MEDLINE | ID: mdl-34830010

RESUMO

Dry eye disease (DED) is one of the major ophthalmological healthcare challenges worldwide. DED is a multifactorial disease characterized by a loss of homeostasis of the tear film, and its main pathogenesis is chronic ocular surface inflammation related with various cellular and molecular signaling cascades. The animal model is a reliable and effective tool for understanding the various pathological mechanisms and molecular cascades in DED. Considerable experimental research has focused on developing new strategies for the prevention and treatment of DED. Several experimental models of DED have been developed, and different animal species such as rats, mice, rabbits, dogs, and primates have been used for these models. Although the basic mechanisms of DED in animals are nearly identical to those in humans, proper knowledge about the induction of animal models is necessary to obtain better and more reliable results. Various experimental models (in vitro and in vivo DED models) were briefly discussed in this review, along with pathologic features, analytical approaches, and common measurements, which will help investigators to use the appropriate cell lines, animal, methods, and evaluation parameters depending on their study design.


Assuntos
Síndromes do Olho Seco/genética , Inflamação/genética , Aparelho Lacrimal/metabolismo , Lágrimas/metabolismo , Animais , Modelos Animais de Doenças , Cães , Síndromes do Olho Seco/patologia , Síndromes do Olho Seco/terapia , Humanos , Inflamação/patologia , Inflamação/terapia , Aparelho Lacrimal/patologia , Camundongos , Coelhos , Ratos
16.
Molecules ; 26(1)2021 Jan 02.
Artigo em Inglês | MEDLINE | ID: mdl-33401664

RESUMO

The formation of amide bonds represents one of the most fundamental processes in organic synthesis. Transition-metal-catalyzed activation of acyclic twisted amides has emerged as an increasingly powerful platform in synthesis. Herein, we report the transamidation of N-activated twisted amides by selective N-C(O) cleavage mediated by air- and moisture-stable half-sandwich Ni(II)-NHC (NHC = N-heterocyclic carbenes) complexes. We demonstrate that the readily available cyclopentadienyl complex, [CpNi(IPr)Cl] (IPr = 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidene), promotes highly selective transamidation of the N-C(O) bond in twisted N-Boc amides with non-nucleophilic anilines. The reaction provides access to secondary anilides via the non-conventional amide bond-forming pathway. Furthermore, the amidation of activated phenolic and unactivated methyl esters mediated by [CpNi(IPr)Cl] is reported. This study sets the stage for the broad utilization of well-defined, air- and moisture-stable Ni(II)-NHC complexes in catalytic amide bond-forming protocols by unconventional C(acyl)-N and C(acyl)-O bond cleavage reactions.


Assuntos
Amidas/química , Ésteres/química , Níquel/química , Compostos Organometálicos/química , Ar , Compostos de Anilina/química , Catálise , Técnicas de Química Sintética , Cinética , Metano/análogos & derivados , Metano/química , Nitrogênio/química
17.
J Med Virol ; 92(6): 632-638, 2020 06.
Artigo em Inglês | MEDLINE | ID: mdl-32124990

RESUMO

There is an obvious concern globally regarding the fact about the emerging coronavirus 2019 novel coronavirus (2019-nCoV) as a worldwide public health threat. As the outbreak of COVID-19 causes by the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) progresses within China and beyond, rapidly available epidemiological data are needed to guide strategies for situational awareness and intervention. The recent outbreak of pneumonia in Wuhan, China, caused by the SARS-CoV-2 emphasizes the importance of analyzing the epidemiological data of this novel virus and predicting their risks of infecting people all around the globe. In this study, we present an effort to compile and analyze epidemiological outbreak information on COVID-19 based on the several open datasets on 2019-nCoV provided by the Johns Hopkins University, World Health Organization, Chinese Center for Disease Control and Prevention, National Health Commission, and DXY. An exploratory data analysis with visualizations has been made to understand the number of different cases reported (confirmed, death, and recovered) in different provinces of China and outside of China. Overall, at the outset of an outbreak like this, it is highly important to readily provide information to begin the evaluation necessary to understand the risks and begin containment activities.


Assuntos
Algoritmos , Betacoronavirus/patogenicidade , Infecções por Coronavirus/epidemiologia , Conhecimentos, Atitudes e Prática em Saúde , Pandemias , Pneumonia Viral/epidemiologia , COVID-19 , Gráficos por Computador , Convalescença , Infecções por Coronavirus/diagnóstico , Infecções por Coronavirus/prevenção & controle , Infecções por Coronavirus/transmissão , Bases de Dados Factuais , Conjuntos de Dados como Assunto , Humanos , Cooperação Internacional , Pandemias/prevenção & controle , Pneumonia Viral/diagnóstico , Pneumonia Viral/prevenção & controle , Pneumonia Viral/transmissão , Saúde Pública/estatística & dados numéricos , SARS-CoV-2 , Análise de Sobrevida
18.
Chemistry ; 26(69): 16246-16250, 2020 Dec 09.
Artigo em Inglês | MEDLINE | ID: mdl-32668046

RESUMO

The structure and properties of amides are of tremendous interest in organic synthesis and biochemistry. Traditional amides are planar and the carbonyl group non-electrophilic due to nN →π*C=O conjugation. In this study, we report electrophilicity scale by exploiting 17 O NMR and 15 N NMR chemical shifts of acyclic twisted and destabilized acyclic amides that have recently received major attention as precursors in N-C(O) cross-coupling by selective oxidative addition as well as precursors in electrophilic activation of N-C(O) bonds. Most crucially, we demonstrate that acyclic twisted amides feature electrophilicity of the carbonyl group that ranges between that of acid anhydrides and acid chlorides. Furthermore, a wide range of electrophilic amides is possible with gradually varying carbonyl electrophilicity by steric and electronic tuning of amide bond properties. Overall, the study quantifies for the first time that steric and electronic destabilization of the amide bond in common acyclic amides renders the amide bond as electrophilic as acid anhydrides and chlorides. These findings should have major implications on the fundamental properties of amide bonds.

19.
J Org Chem ; 85(8): 5475-5485, 2020 04 17.
Artigo em Inglês | MEDLINE | ID: mdl-32159351

RESUMO

N-Acyl-glutarimides have emerged as the most reactive precursors for N-C(O) bond cross-coupling reactions to date, wherein the reactivity is driven by ground-state destabilization of the amide bond. Herein, we report a full study on the effect of a glutarimide ring on the structures, electronic properties, and reactivity of fully perpendicular N-acyl-glutarimide amides. Most notably, this report demonstrates the generality of deploying N-acyl-glutarimides to achieve full twist of the acyclic amide bond, and results in the discovery of N-acyl-glutarimide amide with an almost perfect twist value, τ = 89.1°. X-ray structures of five new N-acyl-glutarimides are reported. Reactivity studies in the Suzuki-Miyaura cross-coupling and transamidation reactions provide insight into the reactivity of N-acyl-glutarimides in metal-catalyzed and transition-metal-free reactions. The effect of distortion, structures, and rotational barriers around the N-C(O) axis is discussed. The ability to achieve full distortion of the amide bond significantly expands the range of reagents available for N-C(O) cross-coupling reactions.

20.
Nanotechnology ; 31(42): 425604, 2020 Jun 08.
Artigo em Inglês | MEDLINE | ID: mdl-32512542

RESUMO

The synthesis of boron nitride nanodisks (BNNDs) with reducing the size and having fewer disk layers, and low optical band gap (E g) is essential for practical applications in electronics and optoelectronic devices. So far, the large-scale preparation of hydroxyl (-OH) and hydroperoxyl (-OOH) functionalized boron nitride nanosheets and BNNDs with reduced E g is still a challenge. This research demonstrates the scalable and solution process synthesis of hydroxyl (-OH) and hydroperoxyl (-OOH) functionalization of BNNDs at the edges and basal planes from pristine hexagonal boron nitride (h-BN) by the combination of modified Hummer's method and Fenton's chemistry. Modified Hummer's method induces exfoliation and cutting of the h-BN into BNNDs with a low percentage of -OH functionalization (6.90%), which is further exfoliated and cut by Fenton's reagent with improved -OH and -OOH functionalization (ca. 17.25%). The combination of these two methods allows us to reduce the size of the OH/OOH-BNNDs to ca. 200 nm with the number of disk layers in the range from ca. 6-11. Concurrently, the E g of h-BN was decreased from ca. 5.10 to ca. 3.58 eV for OH/OOH-BNNDs, which enables the possible application of OH/OOH-BNNDs in semiconductor electronics. The high percentage of -OH and -OOH functionalizations in the OH/OOH-BNNDs enablesg them to disperse in various solvents with high long-term stability.

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