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1.
Physiol Plant ; 176(2): e14249, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-38472657

RESUMEN

The potential of fulvic acid (FA) to improve plant growth has been acknowledged, but its effect on plant growth and nutrient uptake under nutrient stress remains unclear. This study investigated the effects of different FA application rates on maize growth and nitrogen utilization under low nitrogen stress. The results showed that under low nitrogen stress, FA significantly stimulated maize growth, particularly root development, biomass, and nitrogen content. The enhanced activity levels of key enzymes in nitrogen metabolism were observed, along with differential gene expression in maize, which enriched nitrogen metabolism, amino acid metabolism and plant hormone metabolism. The application of FA regulated the hormones' level, reduced abscisic acid content in leaves and Me-JA content in roots, and increased auxin and zeatin ribose content in leaves. This study concludes that, by promoting root development, nitrogen metabolism, and hormone metabolism, an appropriate concentration of FA can enhance plant tolerance to low nitrogen conditions and improve nitrogen use efficiency.


Asunto(s)
Benzopiranos , Nitrógeno , Zea mays , Nitrógeno/metabolismo , Zea mays/metabolismo , Reguladores del Crecimiento de las Plantas/metabolismo , Ácido Abscísico/metabolismo , Raíces de Plantas/metabolismo
2.
Angew Chem Int Ed Engl ; 63(19): e202400122, 2024 May 06.
Artículo en Inglés | MEDLINE | ID: mdl-38494445

RESUMEN

Electrochemical acetylene reduction (EAR) employing Cu catalysts represents an environmentally friendly and cost-effective method for ethylene production and purification. However, Cu-based catalysts encounter product selectivity issues stemming from carbon-carbon coupling and other side reactions. We explored the use of secondary metals to modify Cu-based catalysts and identified Cd decoration as particular effective. Cd decoration demonstrated a high ethylene Faradaic efficiency (FE) of 98.38 % with well-inhibited carbon-carbon coupling reactions (0.06 % for butadiene FE at -0.5 V versus reversible hydrogen electrode) in a 5 vol % acetylene gas feed. Notably, ethylene selectivity of 99.99 % was achieved in the crude ethylene feed during prolonged stability tests. Theoretical calculations revealed that Cd metal accelerates the water dissociation on neighboring Cu surfaces allowing more H* to participate in the acetylene semi-hydrogenation, while increasing the energy barrier for carbon-carbon coupling, thereby contributing to a high ethylene semi-hydrogenation efficiency and significant inhibition of carbon-carbon coupling. This study provides a paradigm for a deeper understanding of secondary metals in regulating the product selectivity of EAR electrocatalysts.

3.
BMC Plant Biol ; 23(1): 54, 2023 Jan 24.
Artículo en Inglés | MEDLINE | ID: mdl-36694111

RESUMEN

BACKGROUND: Sugarcane growth and yield are complex biological processes influenced by endophytic nitrogen-fixing bacteria, for which the molecular mechanisms involved are largely unknown. In this study, integrated metabolomic and RNA-seq were conducted to investigate the interaction between an endophytic bacterial strain, Burkholderia GXS16, and sugarcane tissue culture seedlings. RESULTS: During treatment, the colonization of GXS16 in sugarcane roots were determined, along with the enhanced activities of various antioxidant enzymes. Accordingly, 161, 113, and 37 differentially accumulated metabolites (DAMs) were found in the pairwise comparisons of adjacent stages. In addition, transcriptomic analyses obtained 1,371 (IN-vs-CN), 1,457 (KN-vs-IN), and 365 (LN-vs-KN) differentially expressed genes (DEGs), which were mainly involved in the pathways of glutathione metabolism and carbon metabolism. We then assessed the pattern of metabolite accumulation and gene expression in sugarcane during GXS16 colonization. The results showed that both DAMs and DGEs in the upregulated expression profiles were involved in the flavonoid biosynthesis pathway. Overall, p-coumaroyl-CoA in sugarcane roots transferred into homoeriodictyol chalcone and 5-deoxyleucopelargonidin due to the upregulation of the expression of genes shikimate O-hydroxycinnamoyltransferase (HCT), chalcone synthase (CHS), and phlorizin synthase (PGT1). CONCLUSIONS: This study provides insights into the gene regulatory mechanisms involved in the interaction between GXS16 and sugarcane roots, which will facilitate future applications of endophytic nitrogen-fixing bacteria to promote crop growth.


Asunto(s)
Fenómenos Biológicos , Bacterias Fijadoras de Nitrógeno , Saccharum , Transcriptoma , Regulación de la Expresión Génica de las Plantas
4.
BMC Plant Biol ; 23(1): 573, 2023 Nov 17.
Artículo en Inglés | MEDLINE | ID: mdl-37978424

RESUMEN

BACKGROUND: Drought limits crop growth and is an important issue in commercial sugarcane (Saccharum officinarum) production. Drought tolerance in sugarcane induced by endophytic nitrogen-fixing bacteria is a complex biological process that ranges from altered gene expression and cellular metabolism to changes in growth and productivity. RESULTS: In this study, changes in physiological features and transcriptome related to drought tolerance in sugarcane conferred by the Burkholderia endophytic nitrogen-fixing bacterial strain GXS16 were investigated. Sugarcane samples inoculated with GXS16 exhibited significantly higher leaf relative water content than those without GXS16 inoculation during the drought stages. Sugarcane treated with GXS16 had lower levels of H2O2 and higher levels of abscisic acid than sugarcane not treated with GXS16 in the non-watering groups. Transcriptomic analysis of sugarcane roots identified multiple differentially expressed genes between adjacent stages under different treatments. Moreover, both trend and weighted correlation network analyses revealed that carotenoid biosynthesis, terpenoid backbone biosynthesis, starch and sucrose metabolism, and plant hormone signal transduction strongly contributed to the drought-tolerant phenotype of sugarcane induced by GXS16 treatment. Accordingly, a gene regulatory network including four differentially regulated genes from carotenoid biosynthesis (crtB, crtZ, ZEP and CYP707A) and three genes from terpenoid backbone biosynthesis (dxs, dxr, and PCME) was constructed. CONCLUSIONS: This study provides insights into the molecular mechanisms underlying the application of GXS16 treatment to enhance drought tolerance in sugarcane, which will lay the foundation for crop development and improve productivity.


Asunto(s)
Bacterias Fijadoras de Nitrógeno , Saccharum , Saccharum/metabolismo , Resistencia a la Sequía , Bacterias Fijadoras de Nitrógeno/metabolismo , Peróxido de Hidrógeno/metabolismo , Ácido Abscísico/metabolismo , Sequías , Agua/metabolismo , Regulación de la Expresión Génica de las Plantas
5.
BMC Plant Biol ; 23(1): 601, 2023 Nov 29.
Artículo en Inglés | MEDLINE | ID: mdl-38030995

RESUMEN

BACKGROUND: Lodging seriously affects sugarcane stem growth and sugar accumulation, reduces sugarcane yield and sucrose content, and impedes mechanization. However, the molecular mechanisms underlying sugarcane lodging tolerance remain unclear. In this study, comprehensive transcriptomic and proteomic analyses were performed to explore the differential genetic regulatory mechanisms between upright (GT42) and lodged (GF98-296) sugarcane varieties. RESULTS: The stain test showed that GT42 had more lignin and vascular bundles in the stem than GF98-296. The gene expression analysis revealed that the genes that were differentially expressed between the two varieties were mainly involved in the phenylpropanoid pathway at the growth stage. The protein expression analysis indicated that the proteins that were differentially expressed between the two varieties were related to the synthesis of secondary metabolites, the process of endocytosis, and the formation of aminoacyl-tRNA. Time-series analysis revealed variations in differential gene expression patterns between the two varieties, whereas significant protein expression trends in the two varieties were largely consistent, except for one profile. The expression of CYP84A, 4CL, and CAD from the key phenylpropanoid biosynthetic pathway was enhanced in GT42 at stage 2 but suppressed in GF98-296 at the growth stage. Furthermore, the expression of SDT1 in the nicotinate and nicotinamide metabolism was enhanced in GT42 cells but suppressed in GF98-296 cells at the growth stage. CONCLUSION: Our findings provide reference data for mining lodging tolerance-related genes that are expected to facilitate the selective breeding of sugarcane varieties with excellent lodging tolerance.


Asunto(s)
Saccharum , Transcriptoma , Saccharum/metabolismo , Proteómica , Perfilación de la Expresión Génica , Grano Comestible/genética , Regulación de la Expresión Génica de las Plantas
6.
PLoS Pathog ; 17(1): e1009221, 2021 01.
Artículo en Inglés | MEDLINE | ID: mdl-33471869

RESUMEN

During oropharyngeal candidiasis (OPC), Candida albicans invades and damages oral epithelial cells, which respond by producing proinflammatory mediators that recruit phagocytes to foci of infection. The ephrin type-A receptor 2 (EphA2) detects ß-glucan and plays a central role in stimulating epithelial cells to release proinflammatory mediators during OPC. The epidermal growth factor receptor (EGFR) also interacts with C. albicans and is known to be activated by the Als3 adhesin/invasin and the candidalysin pore-forming toxin. Here, we investigated the interactions among EphA2, EGFR, Als3 and candidalysin during OPC. We found that EGFR and EphA2 constitutively associate with each other as part of a heteromeric physical complex and are mutually dependent for C. albicans-induced activation. Als3-mediated endocytosis of a C. albicans hypha leads to the formation of an endocytic vacuole where candidalysin accumulates at high concentration. Thus, Als3 potentiates targeting of candidalysin, and both Als3 and candidalysin are required for C. albicans to cause maximal damage to oral epithelial cells, sustain activation of EphA2 and EGFR, and stimulate pro-inflammatory cytokine and chemokine secretion. In the mouse model of OPC, C. albicans-induced production of CXCL1/KC and CCL20 is dependent on the presence of candidalysin and EGFR, but independent of Als3. The production of IL-1α and IL-17A also requires candidalysin but is independent of Als3 and EGFR. The production of TNFα requires Als1, Als3, and candidalysin. Collectively, these results delineate the complex interplay among host cell receptors EphA2 and EGFR and C. albicans virulence factors Als1, Als3 and candidalysin during the induction of OPC and the resulting oral inflammatory response.


Asunto(s)
Candida albicans/fisiología , Candidiasis Bucal/patología , Efrina-A2/metabolismo , Células Epiteliales/patología , Orofaringe/patología , Factores de Virulencia/metabolismo , Animales , Candidiasis Bucal/genética , Candidiasis Bucal/metabolismo , Candidiasis Bucal/microbiología , Citocinas/metabolismo , Modelos Animales de Enfermedad , Efrina-A2/genética , Células Epiteliales/metabolismo , Células Epiteliales/microbiología , Receptores ErbB/genética , Receptores ErbB/metabolismo , Humanos , Masculino , Ratones , Ratones Endogámicos BALB C , Ratones Endogámicos C57BL , Orofaringe/metabolismo , Orofaringe/microbiología , Receptor EphA2 , Factores de Virulencia/genética
7.
J Cardiovasc Pharmacol ; 81(6): 445-453, 2023 06 01.
Artículo en Inglés | MEDLINE | ID: mdl-36972559

RESUMEN

ABSTRACT: Lipoprotein(a) [Lp(a)] has become an important component of the residual risk of cardiovascular diseases. Proprotein convertase subtilisin/kexin type 9 (PCSK9) inhibitors display promising effects in controlling Lp(a) levels. However, the effects of different types and dosages of PCSK9 inhibitors on Lp(a) have not been studied in detail. These include 2 monoclonal antibodies, alirocumab and evolocumab, and inclisiran, a small interfering RNA. We searched PubMed, Web of Science, Embase, and Cochrane Library for randomized controlled trials to investigate the efficacy of PCSK9 inhibitors at the Lp(a) level. Although changes in Lp(a) levels were not the primary endpoint in any of these studies, they all described these valuable data. Forty-one randomized controlled trials with 17,601 participants were included, involving 23 unduplicated interventions. Most PCSK9 inhibitors significantly reduced Lp(a) levels compared with placebo. The pairwise comparison demonstrated no significant difference among most PCSK9 inhibitors. However, in the comparison among different dosages of alirocumab, the dosage of 150 mg Q2W showed a significant reduction in Lp(a) levels compared with the dosages of 150, 200, and 300 mg Q4W. In addition, the comparison results demonstrated the significant efficacy of evolocumab 140 mg Q2W compared with alirocumab at a dosage of 150 mg Q4W. The cumulative rank probabilities demonstrated that evolocumab 140 mg Q2W showed the highest efficacy. This study showed that PCSK9 inhibitors reduced Lp(a) levels by up to 25.1%. A biweekly dose of either 140 mg evolocumab or 150 mg alirocumab was the best treatment option. However, the reduction in Lp(a) levels with a single kind of PCSK9 inhibitor alone did not demonstrate sufficient clinical benefit. Therefore, for patients with very high Lp(a) levels who remain at high residual risk in the context of statin administration, it may be acceptable to use a kind of PCSK9 inhibitor, but the clinical benefit needs further investigation.


Asunto(s)
Anticolesterolemiantes , Proproteína Convertasa 9 , Humanos , Inhibidores de PCSK9 , Lipoproteína(a) , Metaanálisis en Red , Subtilisinas , Anticolesterolemiantes/efectos adversos , Ensayos Clínicos Controlados Aleatorios como Asunto
8.
Inorg Chem ; 62(45): 18331-18337, 2023 Nov 13.
Artículo en Inglés | MEDLINE | ID: mdl-37910803

RESUMEN

Here, two isomeric ionic zero-dimensional indium bromide crystals of α (1)/ß (2)-[OPy][InBr4(Phen)] (OPy = N-octylpyridinium; Phen = 1,10-phenanthroline) have been isolated simply by changing the cooling conditions in solvothermal syntheses. Structural comparisons indicate their different supramolecular interactions, which can be confirmed by Hirshfeld surface analyses. The crystal 2 has additional hydrogen bonds and π-π interactions; as a result, the more compact stacking of 2 could result in a 10-fold higher photoluminescence (PL) quantum yield (PLQY) than that of 1. Density functional theory calculations confirm the electron transition from the inorganic moiety to the organic ligand, which provides a further understanding of the optical process. This work provides a new idea for designing PL indium-based halides by understanding the structure-PL relationship.

9.
BMC Cardiovasc Disord ; 23(1): 227, 2023 05 01.
Artículo en Inglés | MEDLINE | ID: mdl-37127585

RESUMEN

BACKGROUND: Familial hypercholesterolemia (FH) leads to high plasma low-density lipoprotein cholesterol (LDL-C) levels and early cardiovascular morbidity and mortality. We treated a pair of siblings with FH. The cardiovascular manifestations in the proband were more severe than those in his elder sister, although they had almost similar LDL-C levels, ages, and lifestyles. Herein, we report the cases of this family to explore the possible causes of clinical phenotypic differences within the same genetic background. CASE PRESENTATION: We treated a 27-year-old male patient and his 30-year-old sister, both with FH. The coronary angiogram in the male patient revealed 80, 70, and 100% stenosis of the initial, distal right coronary artery branch, and left anterior descending branch, respectively, whereas his sister had almost no coronary stenosis. We treated them accordingly and performed family screening. We found that the LDL-C/particle discordance of the proband is much greater than that of his elder sister. In addition, the average size of LDL-C particle in the proband was smaller than that in his sister. CONCLUSIONS: Patients with FH have a much higher risk of premature atherosclerotic cardiovascular disease, but the clinical manifestations are heterogeneous. The smaller LDL particle size may be the underlying cause for different clinical outcomes in this pair of FH cases and be a potential novel indicator for predicting the prognosis of FH.


Asunto(s)
Hiperlipoproteinemia Tipo II , Hermanos , Masculino , Humanos , LDL-Colesterol , Constricción Patológica , Fenotipo
10.
J Labelled Comp Radiopharm ; 66(10): 321-331, 2023 08.
Artículo en Inglés | MEDLINE | ID: mdl-37337654

RESUMEN

The direct electrophilic deuteration of the aromatic moiety in aromatic and aralkyl amines is reported. The acid-catalyzed deuteration is facilitated by deuterated trifluoromethanesulfonic acid, [D]triflic acid, CF3 SO3 D, TfOD, which acts as both the reaction solvent and the source of the deuterium label. The mild conditions enable room temperature hydrogen/deuterium exchange for most of the para-substituted aromatic amine derivatives studied. In addition, short reaction times and a high degree of aromatic deuteration are achieved and isolation of the product is simple. The optical activity of the chiral aralkyl amines studied was preserved.


Asunto(s)
Aminas , Hidrógeno , Deuterio , Medición de Intercambio de Deuterio
11.
Molecules ; 28(9)2023 Apr 27.
Artículo en Inglés | MEDLINE | ID: mdl-37175182

RESUMEN

The use of radiolabeled glucose for PET imaging resulted in the most commonly used tracer in the clinic, 2-deoxy-2-[18F]fluoroglucose (FDG). More recently, other radiolabeled sugars have been reported for various applications, including imaging tumors and infections. Therefore, in this study, we developed a series of fluorine-18-labeled L-rhamnose derivatives as potential PET tracers of various fungal and bacterial strains. Acetyl-protected triflate precursors of rhamnose were prepared and radiolabeled with fluorine-18 followed by hydrolysis to produce L-deoxy [18F]fluororhamnose. The overall radiochemical yield was 7-27% in a 90 min synthesis time with a radiochemical purity of 95%. In vivo biodistribution of the ligands using PET imaging showed that 2-deoxy-2-[18F]fluoro-L-rhamnose is stable for at least up to 60 min in mice and eliminated via renal clearance. The tracer also exhibited minimal tissue or skeletal uptake in healthy mice resulting in a low background signal.


Asunto(s)
Radioisótopos de Flúor , Ramnosa , Ratones , Animales , Distribución Tisular , Línea Celular Tumoral , Tomografía de Emisión de Positrones/métodos , Radiofármacos
12.
Molecules ; 28(5)2023 Mar 04.
Artículo en Inglés | MEDLINE | ID: mdl-36903625

RESUMEN

Bismuth-halide-based inorganic-organic hybrid materials (Bi-IOHMs) are desirable in luminescence-related applications due to their advantages such as low toxicity and chemical stability. Herein, two Bi-IOHMs of [Bpy][BiCl4(Phen)] (1, Bpy = N-butylpyridinium, Phen = 1,10-phenanthroline) and [PP14][BiCl4(Phen)]·0.25H2O (2, PP14 = N-butyl-N-methylpiperidinium), containing different ionic liquid cations and same anionic units, have been synthesized and characterized. Single-crystal X-ray diffraction reveals that compounds 1 and 2 crystallize in the monoclinic space group of P21/c and P21, respectively. They both possess zero-dimensional ionic structures and exhibit phosphorescence at room temperature upon excitation of UV light (375 nm for 1, 390 nm for 2), with microsecond lifetime (24.13 µs for 1 and 95.37 µs for 2). Hirshfeld surface analysis has been utilized to visually exhibit the different packing motifs and intermolecular interactions in 1 and 2. The variation in ionic liquids makes compound 2 have a more rigid supramolecular structure than 1, resulting in a significant enhancement in photoluminescence quantum yield (PLQY), that is, 0.68% for 1 and 33.24% for 2. In addition, the ratio of the emission intensities for compounds 1 and 2 shows a correlation with temperature. This work provides new insight into luminescence enhancement and temperature sensing applications involving Bi-IOHMs.

13.
Molecules ; 28(4)2023 Feb 19.
Artículo en Inglés | MEDLINE | ID: mdl-36838966

RESUMEN

Recently zero-dimensional (0-D) inorganic-organic metal halides (IOMHs) have become a promising class of optoelectronic materials. Herein, we report a new photoluminescent (PL) 0-D antimony(III)-based IOMH single crystal, namely [H2BPZ][SbCl5]·H2O (BPZ = benzylpiperazine). Photophysical characterizations indicate that [H2BPZ][SbCl5]·H2O exhibits singlet/triplet dual-band emission. Density functional theory (DFT) calculations suggest that [H2BPZ][SbCl5]·H2O has the large energy difference between singlet and triplet states, which might induce the dual emission in this compound. Temperature-dependent PL spectra analyses suggest the soft lattice and strong electron-phonon coupling in this compound. Thermogravimetric analysis shows that the water molecules in the lattice of the title crystal could be removed by thermal treatment, giving rise to a dehydrated phase of [H2BPZ][SbCl5]. Interestingly, such structural transformation is accompanied by a reversible PL emission transition between red light (630 nm, dehydrated phase) and yellow light (595 nm, water-containing phase). When being exposed to an environment with 77% relative humidity, the emission color of the dehydrated phase was able to change from red to yellow within 20 s, and the red emission could be restored after reheating. The red to yellow emission switching could be achieved in acetone with water concentration as low as 0.2 vol%. The reversible PL transition phenomenon makes [H2BPZ][SbCl5]·H2O a potential material for luminescent water-sensing.


Asunto(s)
Calor , Hipertermia Inducida , Antimonio , Cloruros , Luminiscencia , Halógenos
14.
J Am Chem Soc ; 144(22): 9554-9558, 2022 06 08.
Artículo en Inglés | MEDLINE | ID: mdl-35639490

RESUMEN

Oxidative coupling and oxidative rearrangement are two of the most common biosynthetic strategies to form diaryl ethers. In contrast, enzymatic diaryl ether generation that proceeds in a nonoxidative manner has not been characterized thus far. Here, we discovered a versatile thioesterase (TE) domain from the nonreducing polyketide synthase (nrPKS) AN7909, which catalyzes diaryl ether formation through a series of successive steps involving esterification, a Smiles rearrangement, and hydrolysis. Further mutations and biochemical analyses with synthetic mimic substrates provide insight into the proposed catalytic process of the TE domain.


Asunto(s)
Éter , Sintasas Poliquetidas , Sintasas Poliquetidas/química , Sintasas Poliquetidas/genética , Tioléster Hidrolasas/química
15.
Chemistry ; 28(37): e202200609, 2022 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-35514119

RESUMEN

Luminescent organic-inorganic metal halides (OIMHs) are well known as a new materials family in recent years. Novel materials and applications of luminescent OIMHs have been explored by changing either the organic component or the metal halide species. Thereinto, the stimuli-responsive (SR) phenomena in OIMHs have drawn much attention recently, for not only their attractive application potential but also the helpfulness in understanding the stability of OIMHs to the external environment. Herein, the luminescent OIMHs that are sensitive to external stimuli including contact, pressure, mechanical grinding, light, heat, and gas molecules, are reviewed, with an emphasis on analyses of the structural change during the SR process. The applications of SR luminescent OIMHs in widespread fields, including gas sensing, information encryption, and rewritable luminescent paper are summarized. Finally, the challenges that deserve to be further explored in this research field are discussed, which provides certain guidance for the future study of SR luminescent OIMHs.


Asunto(s)
Polímeros de Estímulo Receptivo , Luminiscencia , Metales/química
16.
Pharmacol Res ; 181: 106289, 2022 07.
Artículo en Inglés | MEDLINE | ID: mdl-35671922

RESUMEN

Atherosclerosis (AS) is chronic pathological process based on the inflammatory reaction associated with factors including vascular endothelial dysfunction, inflammation, and autoimmunity. Inflammasomes are known to be at the core of the inflammatory response. As a pattern recognition receptor of innate immunity, the NLRP3 inflammasome mediates the secretion of inflammatory factors by activating the Caspase-1, which is important for maintaining the immune system and regulating the gut microbiome, and participates in the occurrence and development of AS. The intestinal microecology is composed of a large number of complex structures of gut microbiota and its metabolites, which play an important role in AS. The gut microbiota and its metabolites regulate the activation of the NLRP3 inflammasome. Targeting the NLRP3 inflammasome and regulating intestinal microecology represent a new direction for the treatment of AS. This paper systematically reviews the interaction between the NLRP3 inflammasome and gut microbiome in AS, strategies for targeting the NLRP3 inflammasome and gut microbiome for the treatment of AS, and provides new ideas for the research and development of drugs for the treatment of AS.


Asunto(s)
Aterosclerosis , Microbioma Gastrointestinal , Microbioma Gastrointestinal/fisiología , Humanos , Inflamasomas , Inflamación/metabolismo , Proteína con Dominio Pirina 3 de la Familia NLR
17.
Nanotechnology ; 33(18)2022 Feb 07.
Artículo en Inglés | MEDLINE | ID: mdl-35042196

RESUMEN

The increasing energy and environmental problems have made clean energy-driven catalysis a hot research topic. Methane is an earth-abundant raw material but difficult to be converted by thermochemical processes. It is of great significance to seek novel strategies to convert methane into high-value chemicals. Herein, we synthesize a series of transition metal catalysts based on layered double hydroxide precursors which were used for photothermal methane nonoxidative coupling reactions. The strong photothermal and chemisorption effects of the derived transition metal nanostructures allow the efficient activation of methane molecules. Among them, alumina-supported metallic Ni and NiCo-alloy catalysts show excellent methane nonoxidative coupling activities, achieved hydrogen production rates of 4816.53µmol g-1h-1and 5130.9µmol g-1h-1, accompanied by liquid fuels production rates of 59.2 mg g-1h-1and 63 mg g-1h-1, respectively. The findings, therefore, provide a new strategy for methane nonoxidative coupling driven by light energy at mild conditions.

18.
Inorg Chem ; 60(23): 17837-17845, 2021 Dec 06.
Artículo en Inglés | MEDLINE | ID: mdl-34738796

RESUMEN

Zero-dimensional (0D) metal halides with solid-state luminescence switching (SSLS) have attracted attention as sensors and luminescent anticounterfeiting. Herein, selective solvent molecule response and accordingly luminescence switching were discovered in 0D [EtPPh3]2[SbCl5] (1, EtPPh3 = ethyltriphenylphosphonium). More than a dozen kinds of solvent molecules have been tested to find out the selection rule for molecule absorption in 1, which is demonstrated to be the size effect of guest molecules. Confirmed by crystal structural analysis, only the solvents with molecular volume less than 22.3 Å3 could be accommodated in 1 leading to the solvatochromic photoluminescence (PL). The mechanism of solvatochromic PL was also deeply studied, which was found to be closely related to the supramolecular interactions between solvent molecules and the host material. Different functional groups of the solvent molecule can affect its strength of hydrogen bonding with [SbCl5]2-, which is crucial for the distortion level of [SbCl5]2- unit and thus results in not only distinct solvatochromic PL but also distinct thermochromic PL. In addition, they all show typical self-trapped exciton triplet emissions. The additional supramolecular interactions from guest molecules can enhance the photoluminescence quantum yield to be as high as 95%.

19.
Angew Chem Int Ed Engl ; 60(43): 23373-23379, 2021 Oct 18.
Artículo en Inglés | MEDLINE | ID: mdl-34402142

RESUMEN

Herein, a new mechanism, namely, crystalline phase recognition (CPR), is proposed for the single-crystal-to-single-crystal (SCSC) transition of metal halides. Chiral ß-[Bmmim]2 SbCl5 (Bmmim=1-butyl-2,3-methylimidazolium) can recognize achiral α-[Bmmim]2 SbCl5 on the basis of a key-lock feature through intercontact of their single crystals, resulting in a domino phase transition (DPT). The concomitant photoluminescence (PL) switching enables observation of the DPT in situ. The liquid eutectic interface, stress-strain transfer, and feasible thermodynamics are key issues for the CPR. DFT calculations and PL measurements revealed that the optical absorption and emission of the isomers mainly originate from [SbCl5 ]2- anions. The structural effects (e.g., supramolecular interactions and [SbCl5 ]2- distortion) on the optical emission are clarified. As a novel type of stimuli response, the CPR-induced DPT and luminescence switching exhibit potential for application in advanced time-resolved information encryption.

20.
Avian Pathol ; 49(3): 211-220, 2020 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-31809574

RESUMEN

As a transcriptional regulator of the classical binary regulatory system, PhoP plays an important role in the life activities of avian pathogenic Escherichia coli (APEC). In previous experiments, we found that the absence of phoP affects APEC biofilm formation and pathogenicity. To further explore the molecular mechanism of phoP regulation of these phenomena, the differentially expressed gene tolC was screened based on phoP-derived transcriptional data, and the specific sequence identity of the PhoP binding sequence was predicted by bioinformatics and verified by electrophoretic mobility shift assay (EMSA). The results showed that PhoP can directly bind to the tolC promoter. On this basis, tolC deletion and complementary strains were constructed. Biofilm formation was quantified by crystal violet staining and rdar morphology change was observed in these strains. Loss of tolC reduced biofilm formation. We also examined pathological changes in organ paraffin sections by challenging chicks with the strains. After loss of tolC, the clinical signs of pericarditis and liver and spleen enlargement in chicks were alleviated, and pathogenicity to the host cells was decreased. Additionally, quantitative real-time polymerase chain reaction (qRT-PCR) analysis revealed that tolC deletion downregulated secA/secB/secE/secY transcript levels, which are part of the type II secretion system secreting virulence effector element. These results indicate that tolC contributes to the phoP-mediated effect on APEC biofilm formation and pathogenicity.


Asunto(s)
Proteínas de la Membrana Bacteriana Externa/metabolismo , Biopelículas/crecimiento & desarrollo , Proteínas de Escherichia coli/metabolismo , Escherichia coli/metabolismo , Proteínas de Transporte de Membrana/metabolismo , Animales , Antibacterianos/farmacología , Proteínas de la Membrana Bacteriana Externa/genética , Pollos , ADN Bacteriano/genética , Farmacorresistencia Bacteriana , Ensayo de Cambio de Movilidad Electroforética , Escherichia coli/genética , Escherichia coli/patogenicidad , Escherichia coli/fisiología , Infecciones por Escherichia coli/microbiología , Infecciones por Escherichia coli/veterinaria , Proteínas de Escherichia coli/genética , Eliminación de Gen , Regulación Bacteriana de la Expresión Génica/fisiología , Hígado/patología , Proteínas de Transporte de Membrana/genética , Análisis de Secuencia por Matrices de Oligonucleótidos
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