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1.
J Am Chem Soc ; 2024 Jul 12.
Artigo em Inglês | MEDLINE | ID: mdl-38993055

RESUMO

The electrocatalytic nitrate reduction reaction (NITRR) holds great promise for purifying wastewater and producing valuable ammonia (NH3). However, the lack of efficient electrocatalysts has impeded the achievement of highly selective NH3 synthesis from the NITRR. In this study, we report the design and synthesis of two polynuclear Co-cluster-based coordination polymers, {[Co2(TCPPDA)(H2O)5]·(H2O)9(DMF)} and {Co1.5(TCPPDA)[(CH3)2NH2]·(H2O)6(DMF)2} (namely, NJUZ-2 and NJUZ-3), which possess distinct coordination motifs with well-defined porosity, high-density catalytic sites, accessible mass transfer channels, and nanoconfined chemical environments. Benefitting from their intriguing multicore metal-organic coordination framework structures, NJUZ-2 and NJUZ-3 exhibit remarkable catalytic activities for the NITRR. At a potential of -0.8 V (vs. RHE) in an H-type cell, they achieve an optimal Faradaic efficiency of approximately 98.5% and high long-term durability for selective NH3 production. Furthermore, the electrocatalytic performance is well maintained even under strongly acidic conditions. When operated under an industrially relevant current density of 469.9 mA cm-2 in a flow cell, a high NH3 yield rate of up to 3370.6 mmol h-1 g-1cat. was observed at -0.5 V (vs. RHE), which is 20.1-fold higher than that obtained in H-type cells under the same conditions. Extensive experimental analyses, in combination with theoretical computations, reveal that the great enhancement of the NITRR activity is attributed to the preferential adsorption of NO3- and the reduction in energy input required for the hydrogenation of *NO3 and *NO2 intermediates.

2.
Cell Discov ; 10(1): 75, 2024 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-38992047

RESUMO

Conventional macrolide-lincosamide-streptogramin B-ketolide (MLSBK) antibiotics are unable to counter the growing challenge of antibiotic resistance that is conferred by the constitutive methylation of rRNA base A2058 or its G2058 mutation, while the presence of unmodified A2058 is crucial for high selectivity of traditional MLSBK in targeting pathogens over human cells. The absence of effective modes of action reinforces the prevailing belief that constitutively antibiotic-resistant Staphylococcus aureus remains impervious to existing macrolides including telithromycin. Here, we report the design and synthesis of a novel series of macrolides, featuring the strategic fusion of ketolide and quinolone moieties. Our effort led to the discovery of two potent compounds, MCX-219 and MCX-190, demonstrating enhanced antibacterial efficacy against a broad spectrum of formidable pathogens, including A2058-methylated Staphylococcus aureus, Streptococcus pneumoniae, Streptococcus pyogenes, and notably, the clinical Mycoplasma pneumoniae isolates harboring A2058G mutations which are implicated in the recent pneumonia outbreak in China. Mechanistic studies reveal that the modified quinolone moiety of MCX-190 establishes a distinctive secondary binding site within the nascent peptide exit tunnel. Structure-activity relationship analysis underscores the importance of this secondary binding, maintained by a sandwich-like π-π stacking interaction and a water-magnesium bridge, for effective engagement with A2058-methylated ribosomes rather than topoisomerases targeted by quinolone antibiotics. Our findings not only highlight MCX-219 and MCX-190 as promising candidates for next-generation MLSBK antibiotics to combat antibiotic resistance, but also pave the way for the future rational design of the class of MLSBK antibiotics, offering a strategic framework to overcome the challenges posed by escalating antibiotic resistance.

3.
J Hazard Mater ; 476: 134909, 2024 Jun 18.
Artigo em Inglês | MEDLINE | ID: mdl-38905979

RESUMO

Developing highly-efficient electrocatalysts for the nitrate reduction reaction (NITRR) is a persistent challenge. Here, we present the successful synthesis of 14 amorphous/low crystallinity metal nanofilms on three-dimensional carbon fibers (M-NFs/CP), including Al, Ti, Mn, Fe, Co, Ni, Cu, Zn, Ag, In, Sn, Pb, Au, or Bi, using rapid thermal evaporation. Among these samples, our study identifies the amorphous Co nanofilm with fine agglomerated Co clusters as the optimal electrocatalyst for NITRR in a neutral medium. The resulting Co-NFs/CP exhibits a remarkable Faradaic efficiency (FENH3) of 91.15 % at - 0.9 V vs RHE, surpassing commercial Co foil (39 %) and Co powder (20 %), despite sharing the same metal composition. Furthermore, during the electrochemical NITRR, the key intermediates on the surface of the Co-NFs/CP catalyst were detected by in situ Fourier-transform infrared (FTIR) spectroscopy, and the possible reaction ways were probed by Density functional theory (DFT) calculations. Theoretical calculations illustrate that the abundant low-coordinate Co atoms of Co-NFs/CP could enhances the adsorption of *NO3 intermediates compared to crystalline Co. Additionally, the amorphous Co structure lowers the energy barrier for the rate-determining step (*NH2→*NH3). This work opens a new avenue for the controllable synthesis of amorphous/low crystallinity metal nano-catalysts for various electrocatalysis reaction applications.

4.
Water Res ; 258: 121774, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38772316

RESUMO

Sustainable and rapid production of high-valent cobalt-oxo (Co(IV)=O) species for efficiently removing organic pollutants is challenging in permoxymonosulfate (PMS) based advanced-oxidation-processes (AOPs) due to the limitation of the high 3d-orbital electronic occupancy of Co and slow conversion from Co(III) to Co(II). Herein, S-scheme BiOCl-OV/CoAl-LDH heterojunction were constructed by ultrathin BiOCl with the oxygen-vacancy (OV) self-assembled with ultrathin CoAl-LDH. OV promoted the formation of charge transfer channel (Bi-O-Co bonds) at the interface of the heterojunction and reduced electron occupation of the Co 3d-orbital to facilitate the generation of Co(IV)=O in the BiOCl-OV/CoAl-LDH/PMS/Visible-light system. S-scheme heterojunction accelerated the photogenerated electrons to allow rapid conversion of Co(III) to Co(II), promoting the fast two-electron transfer from Co(II) to Co(IV)=O. Consequently, the developed BiOCl-OV/CoAl-LDH/PMS/Visible-light system showed excellent degradation efficiency for most of organic pollutions, and exhibited very high removal capability for the actual industrial wastewater. This study provides a new insight into the evolution of Co(IV)=O and the coordinative mechanism for photocatalysis and PMS activation.


Assuntos
Cobalto , Cobalto/química , Catálise , Peróxidos/química , Oxirredução , Poluentes Químicos da Água/química
5.
Org Lett ; 26(22): 4733-4737, 2024 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-38780902

RESUMO

For transition-metal-catalyzed C-H functionalization, precise differentiation between remote adjacent C(sp2)-H bonds remains a long-standing challenge. Here, the template structure-directivity relationship on remote C-H functionalization of arenes was experimentally and computationally studied. By using geometry-tunable templates, Pd-catalyzed remote meta- and para-C-H activation of benzoic acids was achieved with high site selectivity.

6.
ACS Nano ; 18(22): 14020-14028, 2024 Jun 04.
Artigo em Inglês | MEDLINE | ID: mdl-38764286

RESUMO

The electrochemical CO2 reduction reaction (CO2RR) has emerged as a promising approach for sustainable carbon cycling and valuable chemical production. Various methods and strategies have been explored to boost CO2RR performance. One of the most promising strategies includes the construction of stable ionic interfaces on metallic or molecular catalysts using organic or inorganic cations, which has demonstrated a significant improvement in catalytic performance. The stable ionic interface is instrumental in adjusting adsorption behavior, influencing reactive intermediates, facilitating mass transportation, and suppressing the hydrogen evolution reaction, particularly under acidic conditions. In this Perspective, we provide an overview of the recent advancements in building ionic interfaces in the electrocatalytic process and discuss the application of this strategy to improve the CO2RR performance of metallic and molecular catalysts. We aim to convey the future trends and opportunities in creating ionic interfaces to further enhance carbon utilization efficiency and the productivity of CO2RR products. The emphasis of this Perspective lies in the pivotal role of ionic interfaces in catalysis, providing a valuable reference for future research in this critical field.

7.
Heliyon ; 10(9): e29915, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38756596

RESUMO

The control precision of the working device has always been a challenging aspect in unmanned excavator research due to the adoption of a triangular drive mode and a complex hydraulic system in the working mechanism. The article focuses on the research of autonomous control for the downward motion of a robotic arm in an unmanned excavator equipped with a regeneration valve. The study aims to achieve precise tracking of fast movement trajectories during operator manipulation, utilizing Model Predictive Control (MPC). Furthermore, the exceptional disturbance rejection capability of the MPC algorithm is demonstrated through interference application. A comprehensive model considering mechanical, hydraulic, and electrical factors is established for the excavator boom. The MPC algorithm is applied to achieve precise control over the boom descent process, providing a foundation for motion control in unmanned excavators. This article presents a theoretical analysis to elucidate the robustness principle of MPC in the descent control of uncertain dynamic arms. By incorporating real parameters, we successfully track predetermined planned paths at different speeds and validate them on a 20-ton hydraulic excavator. The results demonstrate that the MPC control algorithm accurately manipulates the boom descent motion while exhibiting excellent disturbance rejection performance. Compared to PID control algorithms, MPC offers wider target adaptability range and better disturbance rejection performance, making it suitable for rapid application in controlling working devices of unmanned excavators.

8.
Nutr Diabetes ; 14(1): 31, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38773069

RESUMO

OBJECTIVES: The purpose of this review is to investigate the relationship between gastrointestinal microbiome, obesity, and gestational diabetes mellitus (GDM) in an objective manner. METHODS: We conducted a thorough and comprehensive search of the English language literatures published in PubMed, Web of Science, and the Cochrane Library from the establishment of the library until 12 December 2023. Our search strategy included both keywords and free words searches, and we strictly applied inclusion and exclusion criteria. Meta-analyses and systematic reviews were prepared. RESULTS: Six high-quality literature sources were identified for meta-analysis. However, after detailed study and analysis, a certain degree of heterogeneity was found, and the credibility of the combined analysis results was limited. Therefore, descriptive analyses were conducted. The dysbiosis of intestinal microbiome, specifically the ratio of Firmicutes/Bacteroides, is a significant factor in the development of metabolic diseases such as obesity and gestational diabetes. Patients with intestinal dysbiosis and obesity are at a higher risk of developing GDM. CONCLUSIONS: During pregnancy, gastrointestinal microbiome disorders and obesity may contribute to the development of GDM, with all three factors influencing each other. This finding could aid in the diagnosis and management of patients with GDM through further research on their gastrointestinal microbiome.


Assuntos
Diabetes Gestacional , Disbiose , Microbioma Gastrointestinal , Obesidade , Humanos , Diabetes Gestacional/microbiologia , Gravidez , Feminino , Obesidade/microbiologia , Disbiose/microbiologia
9.
Gut Microbes ; 16(1): 2347728, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38706226

RESUMO

Indole in the gut is formed from dietary tryptophan by a bacterial tryptophan-indole lyase. Indole not only triggers biofilm formation and antibiotic resistance in gut microbes but also contributes to the progression of kidney dysfunction after absorption by the intestine and sulfation in the liver. As tryptophan is an essential amino acid for humans, these events seem inevitable. Despite this, we show in a proof-of-concept study that exogenous indole can be converted to an immunomodulatory tryptophan metabolite, indole-3-lactic acid (ILA), by a previously unknown microbial metabolic pathway that involves tryptophan synthase ß subunit and aromatic lactate dehydrogenase. Selected bifidobacterial strains converted exogenous indole to ILA via tryptophan (Trp), which was demonstrated by incubating the bacterial cells in the presence of (2-13C)-labeled indole and l-serine. Disruption of the responsible genes variedly affected the efficiency of indole bioconversion to Trp and ILA, depending on the strains. Database searches against 11,943 bacterial genomes representing 960 human-associated species revealed that the co-occurrence of tryptophan synthase ß subunit and aromatic lactate dehydrogenase is a specific feature of human gut-associated Bifidobacterium species, thus unveiling a new facet of bifidobacteria as probiotics. Indole, which has been assumed to be an end-product of tryptophan metabolism, may thus act as a precursor for the synthesis of a host-interacting metabolite with possible beneficial activities in the complex gut microbial ecosystem.


Assuntos
Bifidobacterium , Microbioma Gastrointestinal , Indóis , Triptofano , Triptofano/metabolismo , Humanos , Indóis/metabolismo , Bifidobacterium/metabolismo , Bifidobacterium/genética , Triptofano Sintase/metabolismo , Triptofano Sintase/genética , Trato Gastrointestinal/microbiologia , Trato Gastrointestinal/metabolismo
10.
Chem Soc Rev ; 53(10): 5149-5189, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38566609

RESUMO

The electrochemical reduction of CO2 into value-added chemicals has been explored as a promising solution to realize carbon neutrality and inhibit global warming. This involves utilizing the electrochemical CO2 reduction reaction (CO2RR) to produce a variety of single-carbon (C1) and multi-carbon (C2+) products. Additionally, the electrolyte solution in the CO2RR system can be enriched with nitrogen sources (such as NO3-, NO2-, N2, or NO) to enable the synthesis of organonitrogen compounds via C-N coupling reactions. However, the electrochemical conversion of CO2 into valuable chemicals still faces challenges in terms of low product yield, poor faradaic efficiency (FE), and unclear understanding of the reaction mechanism. This review summarizes the promising strategies aimed at achieving selective production of diverse carbon-containing products, including CO, formate, hydrocarbons, alcohols, and organonitrogen compounds. These approaches involve the rational design of electrocatalysts and the construction of coupled electrocatalytic reaction systems. Moreover, this review presents the underlying reaction mechanisms, identifies the existing challenges, and highlights the prospects of the electrosynthesis processes. The aim is to offer valuable insights and guidance for future research on the electrocatalytic conversion of CO2 into carbon-containing products of enhanced value-added potential.

11.
Angew Chem Int Ed Engl ; 63(24): e202405310, 2024 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-38606567

RESUMO

Chiral hybrid metal halides hold great potential as circularly polarized luminescence light sources. Herein, we have obtained two enantiomeric pairs of one-dimensional hybrid chiral manganese(II) chloride single crystals, R/S-(3-methyl piperidine)MnCl3 (R/S-1) and R/S-(3-hydroxy piperidine)MnCl3 (R/S-2), crystallizing in the non-centrosymmetric space group P212121. In comparison to R/S-1, R/S-2 single crystals not only show red emission with near-unity photoluminescence quantum yield (PLQY) and high resistance to thermal quenching but also exhibit circularly polarized luminescence with an asymmetry factor (glum) of 2.5×10-3, which can be attributed to the enhanced crystal rigidity resulting from the hydrogen bonding networks between R/S-(3-hydroxy piperidine) cations and [MnCl6]4- chains. The circularly polarized luminescence activities originate from the asymmetric [MnCl6]4- luminophores induced by N-H⋅⋅⋅Cl hydrogen bonding with R/S-(3-hydroxy piperidine). Moreover, these samples demonstrate great application potential in circularly polarized light-emitting diodes and X-ray scintillators. This work shows a highly efficient photoluminescent Mn-based halide and offers a strategy for designing multifunctional chiral metal halides.

12.
Exp Appl Acarol ; 92(3): 403-421, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38489086

RESUMO

Spider mites (Acari: Tetranychidae) are polyphagous pests of economic importance in agriculture, among which the two-spotted spider mite Tetranychus urticae Koch has spread widely worldwide as an invasive species, posing a serious threat to fruit tree production in China, including Beijing. The hawthorn spider mite, Amphitetranychus viennensis Zacher, is also a worldwide pest of fruit trees and woody ornamental plants. The cassava mite, Tetranychus truncatus Ehara, is mainly found in Asian countries, including China, Korea and Japan, and mainly affects fruit trees and agricultural crops. These three species of spider mites are widespread and serious fruit tree pests in Beijing. Rapid and accurate identification of spider mites is essential for effective pest and plant quarantine in Beijing orchard fields. The identification of spider mite species is difficult due to their limited morphological characteristics. Although the identification of insect and mite species based on PCR and real-time polymerase chain reaction TaqMan is becoming increasingly common, DNA extraction is difficult, expensive and time-consuming due to the minute size of spider mites. Therefore, the objective of this study was to establish a direct multiplex PCR method for the simultaneous identification of three common species of spider mites in orchards, A. viennensis, T. truncatus and T. urticae, to provide technical support for the differentiation of spider mite species and phytosanitary measures in orchards in Beijing. Based on the mitochondrial cytochrome c oxidase subunit I (COI) of the two-spotted spider mite and the cassava mite and the 18S gene sequence of the hawthorn spider mite as the amplification target, three pairs of specific primers were designed, and the primer concentrations were optimized to establish a direct multiplex PCR system for the rapid and accurate discrimination of the three spider mites without the need for DNA extraction and purification. The method showed a high sensitivity of 0.047 ng for T. truncatus and T. urticae DNA and 0.0002 ng for A. viennensis. This method eliminates the DNA extraction and sequencing procedures of spider mite samples, offers a possibility for rapid monitoring of multiple spider mites in an integrated microarray laboratory system, reducing the time and cost of leaf mite identification and quarantine monitoring in the field.


Assuntos
Reação em Cadeia da Polimerase Multiplex , Tetranychidae , Animais , Tetranychidae/genética , Reação em Cadeia da Polimerase Multiplex/métodos , Pequim , Complexo IV da Cadeia de Transporte de Elétrons/genética
13.
Water Res ; 254: 121399, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38447375

RESUMO

Despite numerous studies investigating the occurrence and fate of microplastics, no effort has been devoted toward exploring the characteristics of dissolved organic matter (DOM) leached from face masks mainly made of plastics and additives used in large quantities during the COVID-19 pandemic. By using FTIR, UV-vis, fluorescence EEM coupling with FRI and PARAFAC, and kinetic models of leaching experiments, we explored the leaching behaviors of face mask-derived DOM (FM-DOM) from commonly used face masks including N95, KN95, medical surgical masks, etc. The concentration of FM-DOM increased quickly at early 0-48 h and reached equilibrium at about 48 h measured in terms of dissolved organic carbon and fluorescence intensity. The protein-like materials ranged from 80.32 % to 89.40 % of percentage fluorescence response (Pi,n) were dominant in four types of FM-DOM analyzed by fluorescence EEM-FRI during the leaching experiments from 1 to 360 h. Four fluorescent components were identified, which included tryptophan-like components, tyrosine-like components, microbial protein-like components, and fulvic-like components with fluorescence EEM-PARAFAC models. The multi-order kinetic model (Radj2 0.975-0.999) fitted better than the zero-order and first-order kinetic model (Radj2 0.936-0.982) for all PARAFAC components of FM-DOM based on equations derived by pseudo kinetic models. The leaching rate constants (kn) ranged from 0.058 to 30.938 and the half-life times (T1/2) ranged from 2.73 to 24.87 h for four FM-DOM samples, following the solubility order of fulvic-like components (C4) > microbial protein-like components (C3) > tryptophan-like components (C1) > tyrosine-like components (C2) for FM-DOM from four types of face masks during the leaching experiment from 0 to 360 h. These novel findings will contribute to the understanding of the underappreciated environment impact of face masks in aquatic ecosystems.


Assuntos
Matéria Orgânica Dissolvida , Plásticos , Humanos , Ecossistema , Máscaras , Pandemias , Triptofano , Espectrometria de Fluorescência , Tirosina , Substâncias Húmicas/análise , Análise Fatorial
14.
ACS Appl Mater Interfaces ; 16(13): 16399-16407, 2024 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-38527861

RESUMO

Composition screening and structure optimization are two critical factors in improving the electrocatalytic performance of hybrid materials. Herein, we present a straightforward hydrothermal hydrolyzation-topological transformation strategy for the synthesis of a range of Ni-Co bimetallic compounds with a hollow nanoflower structure. Among these Ni-Co compounds, Ni2P/Co2P hollow nanoflowers (HNFs) exhibit the most impressive electrocatalytic activity for the hydrogen evolution reaction (HER), necessitating only an 153 mV overpotential to achieve a current density of 10 mA cm-2 under alkaline conditions. Importantly, this performance remains stable for over 48 h, indicating exceptional durability. The exceptional catalytic performance of Ni2P/Co2P HNFs arises from the synergy between the hybrid Ni2P/Co2P components and the hollow nanoflower structure. The former provides abundant catalytic sites, while electron rearrangement at the heterointerfaces enhances the adsorption/desorption of active species and facilitates electron transfer. The latter contributes to the exposure of catalytic sites, shortening mass and charge transfer routes, and bolstering structural stability during prolonged electrocatalysis. This research offers valuable insights into the screening and optimization of advanced hybrid electrocatalysts, holding significant promise for applications in the emerging field of new energy technologies.

15.
J Am Chem Soc ; 146(13): 9385-9394, 2024 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-38512124

RESUMO

The shuttling of polysulfides on the cathode and the uncontrollable growth of lithium dendrites on the anode have restricted the practical application of lithium-sulfur (Li-S) batteries. In this study, a metal-coordinated 3D covalent organic framework (COF) with a homogeneous distribution of nickel-bis(dithiolene) and N-rich triazine centers (namely, NiS4-TAPT) was designed and synthesized, which can serve as bifunctional hosts for both sulfur cathodes and lithium anodes in Li-S batteries. The abundant Ni centers and N-sites in NiS4-TAPT can greatly enhance the adsorption and conversion of the polysulfides. Meanwhile, the presence of Ni-bis(dithiolene) centers enables uniform Li nucleation at the Li anode, thereby suppressing the growth of Li dendrites. This work demonstrated the effectiveness of integrating catalytic and adsorption sites to optimize the chemical interactions between host materials and redox-active intermediates, potentially facilitating the rational design of metal-coordinated COF materials for high-performance secondary batteries.

16.
ACS Appl Mater Interfaces ; 16(10): 12907-12915, 2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38412035

RESUMO

The practical application of Li-S batteries (LSBs) has long been impeded by the inefficient utilization of sulfur and slow kinetics. Utilizing conductive carbonaceous frameworks as a host scaffold presents an efficient and cost-effective approach to enhance sulfur utilization for redox reactions in LSBs. However, the interaction of pure carbon materials with lithium polysulfide intermediates (LiPSs) is limited to weak van der Waals forces. Hence, the development of an economical method for synthesizing heteroatom-doped carbon materials for sulfur fixation is of paramount importance. In this study, we introduce a hierarchical porous nitrogen-doped carbon sponge (NPCS) with an exceptionally high BET surface area of 3182.2 m2 g-1, achieved through a facile template-assisted polymerization method. The incorporation of inorganic salts, free radical polymerization, and deuteric freeze-drying techniques facilitates the formation of hierarchical pores within the NPCS. After sulfur fixation, the resulting S/NPCS electrode demonstrates remarkable electrochemical performance in LSBs. Specifically, it achieves an 80% sulfur utilization rate, maintains a high reversible specific capacity of 400 mA h g-1 even after 600 cycles at a demanding current density of 5.0 A g-1, and exhibits superior rate capability. It is believed that this work will inspire the rational design of cost-effective carbon-based electrodes for high-performance LSBs.

17.
J Am Chem Soc ; 146(10): 7018-7028, 2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38412508

RESUMO

Aqueous rechargeable magnesium batteries hold immense potential for intrinsically safe, cost-effective, and sustainable energy storage. However, their viability is constrained by a narrow voltage range and suboptimal compatibility between the electrolyte and electrodes. Herein, we introduce an innovative ternary deep eutectic Mg-ion electrolyte composed of MgCl2·6H2O, acetamide, and urea in a precisely balanced 1:1:7 molar ratio. This formulation was optimized by leveraging competitive solvation effects between Mg2+ ions and two organic components. The full batteries based on this ternary eutectic electrolyte, Mn-doped sodium vanadate (Mn-NVO) anode, and copper hexacyanoferrate cathode exhibited an elevated voltage plateau and high rate capability and showcased stable cycling performance. Ex-situ characterizations unveiled the Mg2+ storage mechanism of Mn-NVO involving initial extraction of Na+ followed by subsequent Mg2+ intercalation/deintercalation. Detailed spectroscopic analyses illuminated the formation of a pivotal solid-electrolyte interphase on the anode surface. Moreover, the solid-electrolyte interphase demonstrated a dynamic adsorption/desorption behavior, referred to as the "breathing effect", which substantially mitigated undesired dissolution and side reactions of electrode materials. These findings underscore the crucial role of rational electrolyte design in fostering the development of a favorable solid-electrolyte interphase that can significantly enhance compatibility between electrode materials and electrolytes, thus propelling advancements in aqueous multivalent-ion batteries.

18.
Food Chem ; 445: 138756, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38394906

RESUMO

Biomimetic methods are invariably employed to synthesize hybrid organic-inorganic multilevel structure nanoflowers with self-assembly processes in aqueous solutions, which is an ideal way to meet the challenges of immobilizing antibodies or enzymes in nanomaterial based enzyme-linked immunosorbent assay (nano-ELISA). In this study, we developed protein-inorganic hybrid 3D nanoflowers composed of bovine serum albumin (BSA), horseradish peroxidase (HRP)-conjugated goat anti-mouse IgG (IgG-HRP) and copper(Ⅱ) phosphate (BSA-(IgG-HRP)-Cu3(PO4)2) using a self-assembly biomimetic method. The preparation process avoided the use of any organic solvent and protein immobilization did not require covalent modifications. Additionally, the unique hierarchical structure enhances the thermal and storage stability of HRP. The BSA-(IgG-HRP)-Cu3(PO4)2 hybrid 3D nanoflower was then applied to a nano-ELISA platform for pyridaben detection, achieving a 50% inhibition concentration of 3.90 ng mL-1. The nano-ELISA achieved excellent accuracy for pyridaben detection. Such a novel BSA-(IgG-HRP)-Cu3(PO4)2 hybrid 3D nanoflower provide an excellent reagent for small molecule immunoassay.


Assuntos
Cobre , Nanoestruturas , Piridazinas , Cobre/química , Nanoestruturas/química , Peroxidase do Rábano Silvestre/química , Ensaio de Imunoadsorção Enzimática , Soroalbumina Bovina
19.
Plant Dis ; 2024 Feb 22.
Artigo em Inglês | MEDLINE | ID: mdl-38386300

RESUMO

The genus Passiflora, commonly known as passion fruit, originated in South America, is an economically important horticulture crop and widely distributed in the tropics and subtropics. Yellow passion fruit (Passiflora edulis f. flavicarpa) and purple passion fruit (Passiflora edulis f. edulis) are the two most planted species (Santos-Jiménez et al., 2022), which have been largely cultivated in southern China. The average annual production reaches 600,000 tons, of which yellow fruit accounts for more than 70% (Zhou et al., 2022). In 2022 to 2023, a disease caused flower rot severely in passion fruit plantations. The incidence rate was generally 10% in purple passion fruit, with an incidence up to 60% in yellow passion fruit 'Qinmi No. 9'. Flower rot occurs mainly in the rainy season, especially during periods of prolonged rain. Infected flowers had black patches that were water-soaked on the interior of the flower bud. The patches covered the entire flower bud, and fluffy mycelium and sporangia developed, which caused the flower bud rotten and abscised easily. Five symptomatic flowers from Wuhua, Guangdong (23°23'N, 115°18'E) and 8 symptomatic flowers from Shangsi, Guangxi (21°15'N, 107°98'E) of 'Qinmi No. 9' were collected during flowering period in 2022 and 2023. Diseased flower pieces were surface-sterilized with 70% ethanol for 2 to 3 min, rinsed with sterile distilled water 3 times, and placed on PDA medium at 25℃ in darkness. Four and 6 fungal isolates with similar morphology were isolated from the infected samples of Wuhua and Shangsi, respectively. Two isolates, PRFJ01 from Wuhua and PRGX02 from Shangsi, were randomly selected for further study. Purified fungal colonies at the age of 3 days accompany with diffuse cottony mycelia, turned white to gray later. The mycelia were hyaline and aseptate. Sporangiophores with 0.56 (0.22~1.10) mm in length and 6.1 (3.18~10.87) µm in width (n=100) were erect, light brown, and had rhizoids and stolons at their bases. Sporangia with 48.0 (23.45~92.85) µm in diameter (n=100) were dark-colored, near spherical and having dark ovoid sporangiospores with 3.56 (2.34~6.39) µm × 2.82 (1.73~4.70) µm (n=100). The morphology of the fungus were identical to Rhizopus stolonifer (Ehrenb.) Vuill (Haque et al. 2023). The two isolates were molecularly identified using genomic regions of 28S large ribosomal subunit (LSU) with NL1 and LR3 primers (Cruz-Lachica et al., 2018). The phylogenetic trees revealed the sequences of PRFJ01 (OR801560.1) and PRGX02 (OR801561.1) were 100% and 99% identical to R. stolonifer (MK705761.1 and KC412868.1), respectively. Pathogenicity tests were conducted on healthy flowers and leaves of 5-month-old grafted 'Qinmi No. 9' plants. Mycelial plugs with 5-mm diameter were placed on the flowers and leaves. Three plants were performed for each of the isolates, and the test was repeated twice. The inoculated plants were moisturized with plastic bags. Healthy flowers and leaves inoculated with sterile PDA plugs were used as control. Typical symptoms were observed on inoculated plants after 2 days. The dark grey mycelia and sporangia covered the entire flower after 4 days inoculation. The flower bud became putrid and the flower stalk split off. Lesions on leaves expanded accompany with numerous aerial mycelium. However, the controls were symptomless. R. stolonifer was reisolated from inoculated tissues. Previously, flower rot on passion fruit caused by R. stolonifer has only been recorded in Brazil (Ploetz, 2003). To our knowledge, this is the first report of R. stolonifer causing flower rot on passion fruit in China.

20.
Chin J Nat Med ; 22(1): 62-74, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-38278560

RESUMO

Pathological vascular remodeling is a hallmark of various vascular diseases. Previous research has established the significance of andrographolide in maintaining gastric vascular homeostasis and its pivotal role in modulating endothelial barrier dysfunction, which leads to pathological vascular remodeling. Potassium dehydroandrographolide succinate (PDA), a derivative of andrographolide, has been clinically utilized in the treatment of inflammatory diseases precipitated by viral infections. This study investigates the potential of PDA in regulating pathological vascular remodeling. The effect of PDA on vascular remodeling was assessed through the complete ligation of the carotid artery in C57BL/6 mice. Experimental approaches, including rat aortic primary smooth muscle cell culture, flow cytometry, bromodeoxyuridine (BrdU) incorporation assay, Boyden chamber cell migration assay, spheroid sprouting assay, and Matrigel-based tube formation assay, were employed to evaluate the influence of PDA on the proliferation and motility of smooth muscle cells (SMCs). Molecular docking simulations and co-immunoprecipitation assays were conducted to examine protein interactions. The results revealed that PDA exacerbates vascular injury-induced pathological remodeling, as evidenced by enhanced neointima formation. PDA treatment significantly increased the proliferation and migration of SMCs. Further mechanistic studies disclosed that PDA upregulated myeloid differentiation factor 88 (MyD88) expression in SMCs and interacted with T-cadherin (CDH13). This interaction augmented proliferation, migration, and extracellular matrix deposition, culminating in pathological vascular remodeling. Our findings underscore the critical role of PDA in the regulation of pathological vascular remodeling, mediated through the MyD88/CDH13 signaling pathway.


Assuntos
Caderinas , Lesões das Artérias Carótidas , Diterpenos , Lesões do Sistema Vascular , Camundongos , Ratos , Animais , Fator 88 de Diferenciação Mieloide/genética , Fator 88 de Diferenciação Mieloide/metabolismo , Remodelação Vascular , Proliferação de Células , Lesões do Sistema Vascular/metabolismo , Lesões do Sistema Vascular/patologia , Lesões das Artérias Carótidas/patologia , Simulação de Acoplamento Molecular , Músculo Liso Vascular , Movimento Celular , Camundongos Endogâmicos C57BL , Transdução de Sinais , Succinatos/metabolismo , Succinatos/farmacologia , Potássio/metabolismo , Potássio/farmacologia , Células Cultivadas
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