Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 193
Filtrar
Más filtros

Banco de datos
País/Región como asunto
Tipo del documento
Intervalo de año de publicación
1.
Mol Cell ; 69(2): 334-346.e4, 2018 01 18.
Artículo en Inglés | MEDLINE | ID: mdl-29307513

RESUMEN

Visualizing dynamics of kinase activity in living animals is essential for mechanistic understanding of cell and developmental biology. We describe GFP-based kinase reporters that phase-separate upon kinase activation via multivalent protein-protein interactions, forming intensively fluorescent droplets. Called SPARK (separation of phases-based activity reporter of kinase), these reporters have large dynamic range (fluorescence change), high brightness, fast kinetics, and are reversible. The SPARK-based protein kinase A (PKA) reporter reveals oscillatory dynamics of PKA activities upon G protein-coupled receptor activation. The SPARK-based extracellular signal-regulated kinase (ERK) reporter unveils transient dynamics of ERK activity during tracheal metamorphosis in live Drosophila. Because of intensive brightness and simple signal pattern, SPARKs allow easy examination of kinase signaling in living animals in a qualitative way. The modular design of SPARK will facilitate development of reporters of other kinases.


Asunto(s)
Imagen Óptica/métodos , Fosfotransferasas/fisiología , Transducción de Señal/fisiología , Animales , Proteínas Quinasas Dependientes de AMP Cíclico/metabolismo , Drosophila , Activación Enzimática , Quinasas MAP Reguladas por Señal Extracelular/metabolismo , Proteínas Fluorescentes Verdes/metabolismo , Humanos , Sistema de Señalización de MAP Quinasas/fisiología , Fosforilación , Fosfotransferasas/metabolismo
2.
Langmuir ; 40(22): 11460-11469, 2024 Jun 04.
Artículo en Inglés | MEDLINE | ID: mdl-38780242

RESUMEN

Improving the morphological structure of active materials is a reliable strategy for the fabrication of high-performance supercapacitor electrodes. In this study, we introduce a feasible approach to constructing the graphene/polypyrrole (PPy) composite film implanted onto the current collector through a two-step electrochemical deposition method utilizing MnO2 as an intermediary template. The reduced graphene oxide (rGO) hydrogel film is first hydrothermally grown on a carbon cloth (CC) substrate to obtain a porous rGO@CC electrode on which MnO2 is electrodeposited. Then the as-prepared rGO/MnO2@CC electrode is subjected to the electrochemical polymerization of pyrrole, with MnO2 acting as an oxidizing template to facilitate the oxidative polymerization of pyrrole, ultimately yielding an rGO/PPy composite film on CC. The PPy synthesized via this methodology exhibits a distinctive interconnected structure, resulting in superior electrochemical performance compared with the electrode with PPy directly electrodeposited on rGO@CC. The optimized electrode achieves an impressive specific capacitance of 583.6 F g-1 at 1 A g-1 and retains 83% of its capacitance at 20 A g-1, with a capacitance loss of only 9.5% after 5000 charge-discharge cycles. The corresponding all-solid-state supercapacitor could provide a high energy density of 22.5 Wh kg-1 and a power density of 4.6 kW kg-1, with a capacitance retention of 82.7% after 5000 charge-discharge cycles. Furthermore, the device also demonstrates good flexibility performance upon bending at 90 and 180°. This work presents an innovative method for the preparation of carbon material/conducting polymer electrodes with specific structural characteristics and superior performance.

3.
Langmuir ; 40(2): 1399-1407, 2024 Jan 16.
Artículo en Inglés | MEDLINE | ID: mdl-38164769

RESUMEN

The facile and cost-effective preparation of supercapacitor electrodes is significant for the application of this kind of electrochemical energy-storing module. In this work, we designed a feasible strategy to fabricate a binary active material onto a current collector in one step. A colloidal mixture of graphene oxide and pyrrole layered on a carbon cloth could undergo a redox reaction through a mild hydrothermal process to yield a reduced graphene oxide/polypyrrole hydrogel film anchored onto the carbon cloth. The integrated electrode with the porous graphene/polypyrrole active material could be directly utilized as a freestanding working electrode for electrochemical measurements and the assembly of supercapacitor devices. The as-prepared electrode could achieve a high capacitance of 1221 mF cm-2 at 1 mA cm-2 (531 F g-1) with satisfactory cycling stability. The constructed symmetric supercapacitor with two optimal electrodes could provide an energy density of 70.4 µWh cm-2 (15.3 Wh kg-1). This work offers a feasible pathway toward the integration of graphene/conducting polymer composites as electrochemical electrodes.

4.
Environ Sci Technol ; 58(33): 14831-14842, 2024 Aug 20.
Artículo en Inglés | MEDLINE | ID: mdl-39120612

RESUMEN

There have been numerous studies using effect-directed analysis (EDA) to identify key toxic substances present in source and drinking water, but none of these studies have considered the effects of metabolic activation. This study developed a comprehensive method including a pretreatment process based on an in vitro metabolic activation system, a comprehensive biological effect evaluation based on concentration-dependent transcriptome (CDT), and a chemical feature identification based on nontarget chemical analysis (NTA), to evaluate the changes in the toxic effects and differences in the chemical composition after metabolism. Models for matching metabolites and precursors as well as data-driven identification methods were further constructed to identify toxic metabolites and key toxic precursor substances in drinking water samples from the Yangtze River. After metabolism, the metabolic samples showed a general trend of reduced toxicity in terms of overall biological potency (mean: 3.2-fold). However, metabolic activation led to an increase in some types of toxic effects, including pathways such as excision repair, mismatch repair, protein processing in endoplasmic reticulum, nucleotide excision repair, and DNA replication. Meanwhile, metabolic samples showed a decrease (17.8%) in the number of peaks and average peak area after metabolism, while overall polarity, hydrophilicity, and average molecular weight increased slightly (10.3%). Based on the models for matching of metabolites and precursors and the data-driven identification methods, 32 chemicals were efficiently identified as key toxic substances as main contributors to explain the different transcriptome biological effects such as cellular component, development, and DNA damage related, including 15 industrial compounds, 7 PPCPs, 6 pesticides, and 4 natural products. This study avoids the process of structure elucidation of toxic metabolites and can trace them directly to the precursors based on MS spectra, providing a new idea for the identification of key toxic pollutants of metabolites.


Asunto(s)
Transcriptoma , Contaminantes Químicos del Agua , Contaminantes Químicos del Agua/toxicidad , Activación Metabólica , Agua Potable/química
5.
Environ Sci Technol ; 58(23): 9925-9944, 2024 Jun 11.
Artículo en Inglés | MEDLINE | ID: mdl-38820315

RESUMEN

Organic contaminants are ubiquitous in the environment, with mounting evidence unequivocally connecting them to aquatic toxicity, illness, and increased mortality, underscoring their substantial impacts on ecological security and environmental health. The intricate composition of sample mixtures and uncertain physicochemical features of potential toxic substances pose challenges to identify key toxicants in environmental samples. Effect-directed analysis (EDA), establishing a connection between key toxicants found in environmental samples and associated hazards, enables the identification of toxicants that can streamline research efforts and inform management action. Nevertheless, the advancement of EDA is constrained by the following factors: inadequate extraction and fractionation of environmental samples, limited bioassay endpoints and unknown linkage to higher order impacts, limited coverage of chemical analysis (i.e., high-resolution mass spectrometry, HRMS), and lacking effective linkage between bioassays and chemical analysis. This review proposes five key advancements to enhance the efficiency of EDA in addressing these challenges: (1) multiple adsorbents for comprehensive coverage of chemical extraction, (2) high-resolution microfractionation and multidimensional fractionation for refined fractionation, (3) robust in vivo/vitro bioassays and omics, (4) high-performance configurations for HRMS analysis, and (5) chemical-, data-, and knowledge-driven approaches for streamlined toxicant identification and validation. We envision that future EDA will integrate big data and artificial intelligence based on the development of quantitative omics, cutting-edge multidimensional microfractionation, and ultraperformance MS to identify environmental hazard factors, serving for broader environmental governance.


Asunto(s)
Monitoreo del Ambiente , Monitoreo del Ambiente/métodos , Contaminantes Ambientales , Fraccionamiento Químico
6.
Angew Chem Int Ed Engl ; 63(9): e202317892, 2024 Feb 26.
Artículo en Inglés | MEDLINE | ID: mdl-38206554

RESUMEN

Iodination has unlocked new potentials in organic photovoltaics (OPVs). A newly designed and synthesized iodinated non-fullerene acceptor, BO-4I, showcases exceptional excitation delocalization property with the exciton diffusion length increased to 80 nm. The enhanced electron delocalization property is attributed to the larger atomic radius and electron orbit of the iodine atom, which facilitates the formation of intra-moiety excitations in the acceptor phase. This effectively circumvents the charge transfer state-related recombination mechanisms, leading to a substantial reduction in non-radiative energy loss (ΔEnr ). As a result, OPV cell based on PBDB-TF : BO-4I achieves an impressive efficiency of 18.9 % with a notable ΔEnr of 0.189 eV, markedly surpassing their fluorinated counterparts. This contribution highlights the pivotal role of iodination in reducing energy loss, thereby affirming its potential as a key strategy in the development of advanced next-generation OPV cells.

7.
Angew Chem Int Ed Engl ; 63(15): e202400565, 2024 Apr 08.
Artículo en Inglés | MEDLINE | ID: mdl-38291011

RESUMEN

Organic solar cells (OSCs) are still suffering from the low light utilization and unstable under ultraviolet irradiation. To tackle these challenges, we design and synthesize a non-fused acceptor based on 1-(2-butyloctyl)-1H-pyrrole as π-bridge unit, denoted as GS70, which serves as active layer in the front-cell for constructing tandem OSCs with a parallel configuration. Benefiting from the well-complementary absorption spectra with the rear-cell, GS70-based parallel tandem OSCs exhibit an improved photoelectron response over the range between 600-700 nm, yielding a high short-circuit current density of 28.4 mA cm-2. The improvement in light utilization translates to a power conversion efficiency of 19.4 %, the highest value among all parallel tandem OSCs. Notably, owing to the intrinsic stability of GS70, the manufactured parallel tandem OSCs retain 84.9 % of their initial PCE after continuous illumination for 1000 hours. Overall, this work offers novel insight into the molecular design of low-cost and stability non-fused acceptors, emphasizing the importance of adopting a parallel tandem configuration for achieving efficient light harvesting and improved photostability in OSCs.

8.
Angew Chem Int Ed Engl ; 63(30): e202406153, 2024 Jul 22.
Artículo en Inglés | MEDLINE | ID: mdl-38730419

RESUMEN

Innovative molecule design strategy holds promise for the development of next-generation acceptor materials for efficient organic solar cells with low non-radiative energy loss (ΔEnr). In this study, we designed and prepared three novel acceptors, namely BTP-Biso, BTP-Bme and BTP-B, with sterically structured triisopropylbenzene, trimethylbenzene and benzene as side chains inserted into the shoulder of the central core. The progressively enlarged steric hindrance from BTP-B to BTP-Bme and BTP-Biso induces suppressed intramolecular rotation and altered the molecule packing mode in their aggregation states, leading to significant changes in absorption spectra and energy levels. By regulating the intermolecular π-π interactions, BTP-Bme possesses relatively reduced non-radiative recombination rate and extended exciton diffusion lengths. The binary device based on PB2 : BTP-Bme exhibits an impressive power conversion efficiency (PCE) of 18.5 % with a low ΔEnr of 0.19 eV. Furthermore, the ternary device comprising PB2 : PBDB-TF : BTP-Bme achieves an outstanding PCE of 19.3 %. The molecule design strategy in this study proposed new perspectives for developing high-performance acceptors with low ΔEnr in OSCs.

9.
J Org Chem ; 88(19): 13590-13597, 2023 Oct 06.
Artículo en Inglés | MEDLINE | ID: mdl-37690058

RESUMEN

A novel method for the synthesis of formamides through the decarboxylative N-formylation of amines with glyoxylic acid has been developed. This transformation provides an efficient protocol for the synthesis of various formamides with moderate to excellent yields, and it can accommodate a wide range of functional groups under metal free and base free conditions. In addition, the large-scale experiments and high chemoselectivity have shown great potential application of this strategy.

10.
Inorg Chem ; 62(30): 12067-12078, 2023 Jul 31.
Artículo en Inglés | MEDLINE | ID: mdl-37475677

RESUMEN

LixAg1-xGaSe2 is a new series of solid solution crystals that has a large nonlinear optical (NLO) coefficient and laser-induced damage threshold (LIDT). It has great application prospects in mid-infrared laser frequency conversion. In this work, LixAg1-xGaSe2 (x = 0, 0.2, 0.4, 0.5, 0.6, 0.8, and 1) crystals (Φ 16 mm × 40 mm) were grown by the improved Bridgeman method in a four-zone furnace. It is found that the LixAg1-xGaSe2 (x = 0.2-0.8) crystals keep the same tetragonal symmetry with AgGaSe2 and the melting and solidification temperature increase with the Li content. Because the as-grown crystals are almost opaque in the visible-NIR range, an annealing experiment is necessary. After annealing, the transmittance is improved significantly, which can meet the application requirements. The band gap is changed by annealing atmosphere; for instance, the band gap of Li0.6Ag0.4GaSe2 annealed in a LiGaSe2 powder atmosphere increases from 2.35 to 2.56 eV, while the band gap of LiGaSe2 annealed in vacuum decreases from 3.39 to 3.01 eV. Finally, the LixAg1-xGaSe2 shows an extreme SHG response, especially Li0.8Ag0.2GaSe2, which has about five times that of LiGaSe2, proving the promising NLO properties.

11.
Environ Sci Technol ; 57(51): 21650-21661, 2023 Dec 26.
Artículo en Inglés | MEDLINE | ID: mdl-38078857

RESUMEN

Emerging classes of dioxin-like compounds (DLCs) like hydroxylated/methoxylated polybrominated diphenyl ethers (HO-/MeO-PBDEs) and polychlorinated diphenyl sulfides (PCDPSs) could lead to diverse adverse outcomes in humans and wildlife, yet knowledge gaps exist in their molecular mechanisms associated with different structures following early life environmental exposure. This study integrated a genetic knockout technique and concentration-dependent reduced zebrafish transcriptome approach (CRZT) to unravel the toxicological pathways underpinning developmental toxicity of four HO-/MeO-PBDEs and five PCDPSs at environmentally relevant doses. Generally, the dependence of aryl hydrocarbon receptor (AhR) on the embryotoxicity and transcriptomic potencies induced by the HO-PBDEs and PCDPSs varied across different congeners. The knockout of the ahr2 gene led to 1.02- to 76.48-fold decreases of DLC-induced embryotoxicities and reduced the transcriptome-based potencies ranging from 1.38 to 2124.74 folds in the CRZT test. The fold changes denoting AhR-mediated potentials significantly increased with the increasing chlorination degrees of MeO-PBDEs and PCDPSs (p < 0.05). Moreover, ahr2 knockout primarily affected the DLC-induced early molecular responses relevant to DNA damage, enzyme activation, and organ development. Our integrated approach revealed the differential role of AhR in mediating the developmental toxicity of emerging DLCs possessing varied structures at environmentally relevant doses.


Asunto(s)
Dioxinas , Animales , Humanos , Dioxinas/toxicidad , Éteres Difenilos Halogenados/química , Pez Cebra , Animales Salvajes
12.
Environ Sci Technol ; 57(37): 13744-13756, 2023 09 19.
Artículo en Inglés | MEDLINE | ID: mdl-37677100

RESUMEN

Although previous studies have confirmed the association between phthalate esters (PAEs) exposure and endocrine disorders in humans, few studies to date have systematically assessed the threats of new PAE alternatives to endocrine disruptions. Herein, zebrafish embryos were continuously exposed to two PAEs [di-n-butyl phthalate (DBP) and diisobutyl phthalate (DiBP)], two structurally related alternatives [diiononyl phthalate (DINP) and diisononyl hexahydrophthalate (DINCH)], and two non-PAE substitutes [dipropylene glycol dibenzoate (DGD) and glyceryl triacetate (GTA)], and the endocrine-disrupting effects were investigated during the early stages (8-48 hpf). For five endogenous hormones, including progesterone, testosterone, 17ß-estradiol, triiodothyronine (T3), and cortisol, the tested chemicals disturbed the contents of at least one hormone at environmentally relevant concentrations (≤3.9 µM), except DINCH and GTA. Then, the concentration-dependent reduced zebrafish transcriptome analysis was performed. Thyroid hormone (TH)- and androgen/estrogen-regulated adverse outcome pathways (AOPs) were the two types of biological pathways most sensitive to PAE exposure. Notably, six compounds disrupted four TH-mediated AOPs, from the inhibition of deiodinases (molecular initiating event, MIE), a decrease in T3 levels (key event, KE), to mortality (adverse outcome, AO) with the quantitatively linear relationships between MIE-KE (|r| = 0.96, p = 0.002), KE-AO (|r| = 0.88, p = 0.02), and MIE-AO (|r| = 0.89, p = 0.02). Multiple structural analyses showed that benzoic acid is the critical toxicogenic fragment. Our data will facilitate the screening and development of green alternatives.


Asunto(s)
Dibutil Ftalato , Transcriptoma , Humanos , Animales , Pez Cebra , Ésteres
13.
Environ Res ; 237(Pt 2): 116976, 2023 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-37625535

RESUMEN

Soil, as a heterogeneous body, is composed of different-sized aggregates. There is limited data available on the potential role of microplastics (MPs) in microbial properties at the soil aggregate level. In this study, changes in microbial construction and diversity in farmland bulk soil and aggregates induced by polyethylene MPs (PE-MPs) were investigated at a dose of 0.5% (w/w) through 16s rDNA sequencing and enzyme activity measurements of different particle size aggregates in incubated soil. The presence of low-dose PE-MPs increased the proportion of >1 mm soil aggregates fraction, and decreased soil available nitrogen and available phosphorus in bulk soils. Furthermore, low-dose PE-MPs increased bacterial richness and diversity in 1-0.5 and < 0.25 mm fractions and decreased operational taxonomic unit, abundance-based coverage estimator, and Chao1 indices in bulk soil and >1 mm fractions. The levels of predicted functional genes taking part in the biodegradation and metabolism of exogenous substances also increased. At the phylum level, PE-MPs changed the proportion of Proteobacteria and Actinobacteria. The variations in soil aggregate properties were significantly correlated with the bacterial communities' composition and diversity. This study deepens our perception of the soil microenvironment, microbial community composition, and diversity in response to PE-MPs.

14.
Arch Insect Biochem Physiol ; 112(3): e21991, 2023 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-36533994

RESUMEN

The adaptations of omnivorous insects to food are manifested in a multifaceted manner, and the availability of food resources directly determines insect feeding tendencies, which contribute to a complex insect-food relationship and impact insect functionality in the environment. Stable isotope analysis was applied to test the feeding preference and further define the functional role of omnivorous beetles in cropland. Our results confirmed that as an omnivorous beetle, the fungivorous nature of Notoxus trinotatus accounted for a prominent proportion food selection at the adult stage, and more importantly, this dietary feature contributed to the dispersal of the northern corn leaf blight in maize (NLB) during the feeding trials. In addition to the preference for fungi, water supplementation was an essential element extending adult longevity, which directly prolonged the contact time of adults with pathogenic fungi in agricultural fields. Consistent with the herbivorous characteristics of beetles, before the emergence of NLB fungal pathogens, corn tissues served as the main food, which provided the beetles with more opportunities to transmit fungal pathogen propagules. We conclude that the role of N. trinotatus in carrying NLB pathogen is due to its feeding on this plant mycopathogen, and an increased abundance of beetles carrying the pathogen may increase the rate of NLB disease infestation. More focus should be concentrated on the functions of fungivorous beetles, not only as pathogen-transmitting pests, but also as an element among the balanced biotic factors in farmland.


Asunto(s)
Escarabajos , Animales , Escarabajos/microbiología , Zea mays , Insectos , Plantas , Herbivoria
15.
Proc Natl Acad Sci U S A ; 117(25): 13975-13982, 2020 06 23.
Artículo en Inglés | MEDLINE | ID: mdl-32513708

RESUMEN

Arsenic is a toxic pollutant commonly found in the environment. Most of the previous studies on arsenic pollution have primarily focused on arsenic contamination in groundwater. In this study, we examine the impact on human health from atmospheric arsenic on the global scale. We first develop an improved global atmospheric arsenic emission inventory and connect it to a global model (Goddard Earth Observing System [GEOS]-Chem). Model evaluation using observational data from a variety of sources shows the model successfully reproduces the spatial distribution of atmospheric arsenic around the world. We found that for 2005, the highest airborne arsenic concentrations were found over Chile and eastern China, with mean values of 8.34 and 5.63 ng/m3, respectively. By 2015, the average atmospheric arsenic concentration in India (4.57 ng/m3) surpassed that in eastern China (4.38 ng/m3) due to the fast increase in coal burning in India. Our calculation shows that China has the largest population affected by cancer risk due to atmospheric arsenic inhalation in 2005, which is again surpassed by India in 2015. Based on potential exceedance of health-based limits, we find that the combined effect by including both atmospheric and groundwater arsenic may significantly enhance the risks, due to carcinogenic and noncarcinogenic effects. Therefore, this study clearly implies the necessity in accounting for both atmospheric and groundwater arsenic in future management.


Asunto(s)
Contaminantes Atmosféricos/toxicidad , Intoxicación por Arsénico/epidemiología , Arsénico/toxicidad , Salud Global/estadística & datos numéricos , Modelos Estadísticos , Neoplasias/epidemiología , Contaminantes Atmosféricos/análisis , Arsénico/análisis , Atmósfera/química , Exposición a Riesgos Ambientales/estadística & datos numéricos , Monitoreo del Ambiente , Agua Subterránea/química , Humanos , Análisis Espacio-Temporal
16.
Angew Chem Int Ed Engl ; 62(5): e202214088, 2023 Jan 26.
Artículo en Inglés | MEDLINE | ID: mdl-36448216

RESUMEN

To modulate the miscibility between donor and acceptor materials both possessing fully non-fused ring structures, a series of electron acceptors (A4T-16, A4T-31 and A4T-32) with different polar functional substituents were synthesized and investigated. The three acceptors show good planarity, high conformational stability, complementary absorption and energy levels with the non-fused polymer donor (PTVT-BT). Among them, A4T-32 possesses the strongest polar functional group and shows the highest surface energy, which facilitates morphological modulation in the bulk heterojunction (BHJ) blend. Benefiting from the proper morphology control method, an impressive power conversion efficiency (PCE) of approaching 16.0 % and a superior fill factor over 0.795 are achieved in the PTVT-BT : A4T-32-based organic photovoltaic cells with superior photoactive materials price advantage, which represent the highest value for the cells based on the non-fused blend films. Notably, this cell maintains ≈84 % of its initial PCE after nearly 2000 h under the continuous simulated 1-sun-illumination. In addition, the flexible PTVT-BT : A4T-32-based cells were fabricated and delivered a decent PCE of 14.6 %. This work provides an effective molecular design strategy for the non-fused non-fullerene acceptors (NFAs) from the aspect of bulk morphology control in fully non-fused BHJ layers, which is crucial for their practical applications.

17.
Angew Chem Int Ed Engl ; 62(50): e202314362, 2023 Dec 11.
Artículo en Inglés | MEDLINE | ID: mdl-37877452

RESUMEN

Organic photovoltaic (OPV) cells, with highly tunable light-response ranges, offer significant potential for use in driving low-power consumption off-grid electronics in multi-scenarios. However, development of photoactive layer materials that can meet simultaneously the requirements of diverse irradiation conditions is a still challenging task. Herein, a low-cost fully non-fused acceptor (denoted as GS60) featuring well-matched absorption spectra with solar, scattered light and artificial light radiation was designed and synthesized. Systematic characterizations revealed that GS60 possessed outstanding photoelectron properties and ideal morphology, which resulted in reduced voltage loss and suppressed charge recombination. By blending with a non-fused ring polymer PTVT-T, the as-obtained GS60 based OPV cells achieved a good power conversion efficiency (PCE) of 14.1 %, a high value for the cells based on non-fused ring bulk heterojunction. Besides, manufactured large-area OPV modules based on PTVT-T:GS60 yielded PCEs of 11.2 %, 11.8 %, 12.1 %, 23.1 %, and 20.3 % under irradiation of AM 1.5G, natural light of cloudy weather, natural light in shadow, laser and indoor, respectively. The PTVT-T:GS60 devices exhibited considerable potential in terms of improving photostability and reducing material cost. Overall, this work provides novel insight into the molecular design of low-cost non-fused ring acceptors, and extended potential of medium band gap acceptors based OPV cells used in various application scenarios.

18.
Environ Sci Technol ; 56(1): 175-184, 2022 01 04.
Artículo en Inglés | MEDLINE | ID: mdl-34898191

RESUMEN

Biogenic volatile organic compound (BVOC) emissions have long been known to play vital roles in modulating the formation of ozone and secondary organic aerosols (SOAs). While early studies have evaluated their impact globally or regionally, the BVOC emissions emitted from urban green spaces (denoted as U-BVOC emissions) have been largely ignored primarily due to the failure of low-resolution land cover in resolving such processes, but also because their important contribution to urban BVOCs was previously unrecognized. In this study, by utilizing a recently released high-resolution land cover dataset, we develop the first set of emission inventories of U-BVOCs in China at spatial resolutions as high as 1 km. This new dataset resolved densely distributed U-BVOCs in urban core areas. The U-BVOC emissions in megacities could account for a large fraction of total BVOC emissions, and the good agreement of the interannual variations between the U-BVOC emissions and ozone concentrations over certain regions stresses their potentially crucial role in influencing ozone variations. The newly constructed U-BVOC emission inventory is expected to provide an improved dataset to enable the research community to re-examine the modulation of BVOCs on the formation of ozone, SOA, and atmospheric chemistry in urban environments.


Asunto(s)
Contaminantes Atmosféricos , Ozono , Compuestos Orgánicos Volátiles , Contaminantes Atmosféricos/análisis , China , Ozono/análisis , Parques Recreativos
19.
Anal Chem ; 93(28): 9887-9896, 2021 07 20.
Artículo en Inglés | MEDLINE | ID: mdl-34235921

RESUMEN

Molecular switching plays a critical role in biological and displaying systems. Donor-acceptor Stenhouse adducts (DASAs) is a newly re-discovered series of switchable photochromes, and light is the most used approach to control its switching behavior. In this report, we speculated that hydrophobic binding pockets of biologically relevant peptides/proteins could be harnessed to alter its switching behavior without the assistance of light. We designed and synthesized a DASA compound SHA-2, and we demonstrated that the Aß40 species could stabilize SHA-2 in the linear conformation and decrease the rate of molecular switching via fluorescence spectral studies. Moreover, molecular dynamics simulation revealed that SHA-2 could bind to the hydrophobic fragment of the peptide and resulted in substantial changes in the tertiary structure of Aß40 monomer. This structural change is likely to impede the aggregation of Aß40, as evidenced by the results from thioflavin T fluorescence and ProteoStat aggregation detection experiments. We believe that our study opens a new window to alter the switching behavior of DASA via DASA-peptide/protein interactions.


Asunto(s)
Péptidos beta-Amiloides , Simulación de Dinámica Molecular , Interacciones Hidrofóbicas e Hidrofílicas , Fragmentos de Péptidos
20.
Acc Chem Res ; 53(4): 822-832, 2020 Apr 21.
Artículo en Inglés | MEDLINE | ID: mdl-32216329

RESUMEN

ConspectusOver the past few years, the development of new materials has contributed to rapid increases in the power conversion efficiencies (PCEs) of organic photovoltaic (OPV) cells to over 17%, showing great potential for the commercialization of this technology in the near future. At this stage, designing new materials with superior performance and low cost simultaneously is of crucial importance. Chlorinated materials are emerging as new stars with very high PCEs, creating a molecular design trend to replace the most popular fluorinated materials. For example, by using chlorinated non-fullerene acceptors, we recently got a record PCE of 17% for single-junction OPV cells. Firmly based on recent advances, herein we focus on the topic of chlorinated OPV materials, aiming to provide a guideline for further molecular design.In this Account, first, on the basis of most fundamental features of the Cl atom, we highlight the features of chlorinated materials compared with their fluorinated counterparts: (1) Chlorination is more efficient than fluorination in modulating the optical and electrical properties of OPV materials. In many cases, chlorinated materials show lower energy levels and broader absorption spectra than their fluorinated counterparts, which contribute higher output voltages and current densities in the resulting photovoltaic devices. (2) Cl has a large atomic size than F. On one hand, enhanced overlap of π electrons is beneficial for enhancing the intermolecular packing and crystalline property and thus improving the charge transport. On the other hand, if Cl is introduced inappropriately in the backbone or side chain, this feature will cause a more twisted π plane and larger steric hindrance, having negative impacts on the photovoltaic performance of the corresponding materials. (3) Importantly, chlorination is usually chemically cheaper in synthesis, which has the potential to decrease the material cost of OPV cells. Then, we provide a concise review of chlorinated OPV materials, including polymeric and small-molecule donors and non-fullerene acceptors. The photovoltaic performance in various types of OPV cells using chlorinated materials, such as single-junction, tandem, semitransparent, and indoor-light photovoltaic cells is also discussed. For instance, ultranarrow-band-gap chlorinated acceptors can be used to construct highly efficient color-semitransparent OPV cells, and the wide-band-gap chlorinated materials show great potential for fabricating indoor-light photovoltaic devices. Finally, we briefly discuss current questions related to chlorinated OPV materials and highlight the significance of chlorination in future development.

SELECCIÓN DE REFERENCIAS
DETALLE DE LA BÚSQUEDA