Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 77
Filtrar
2.
Chem Sci ; 2024 Sep 16.
Artículo en Inglés | MEDLINE | ID: mdl-39323518

RESUMEN

In-depth insight into the electronic competition principles between inorganic units and organic ligands proves to be extremely challenging for controlling multi-mode emissions in low-dimensional hybrid metal halides (LHMHs). Herein, an efficient blue emission from organic ligand was engineered in (DppyH)2MCl4 (Dppy = diphenyl-2-pyridylphosphine, M = Zn2+, Cd2+) due to the reverse type I band alignment constructed by optically inert units with nd10 shell electrons. By contrast, the optically active [MnCl4]2- with semi-fully filled 3d5 shell electrons prompts the band alignment of type II, resulting in the narrowband green emission of Mn2+, along with an energy transfer from DppyH+ to [MnCl4]2-. Beyond that, the band alignment of (DppyH)SbCl4 is further reversed to type I due to the strong stereochemical activity of 5s2 lone-pair electrons, resulting in the triplet-state (3P1 → 1S0) self-trapped exciton (STE) emission of [SbCl4]-. The conclusion is that the electronic configurations of metal centers govern the optical activity levels of inorganic units, which in turn controls the multi-mode emissions by maneuvering the band alignments. This research provides an enlightening perspective on the multi-mode emissions with tunable photoluminescence and resulting electronic transitions of LHMHs, whose derived emitters can be employed in anti-counterfeiting and information encryption.

3.
Acc Chem Res ; 57(17): 2522-2531, 2024 Sep 03.
Artículo en Inglés | MEDLINE | ID: mdl-39145737

RESUMEN

ConspectusIn the development of 2D metal-organic frameworks (MOFs) and 2D covalent organic frameworks (COFs), obtaining structural details at the atomic level is crucial to understanding their properties and related mechanisms in potential applications. However, since 2D-MOFs and COFs are composed of layered structures and often exhibit sheet-like morphologies, it is challenging to grow large crystals suitable for single-crystal X-ray diffraction (SCXRD). Therefore, ab initio structure determination, which refers to solving the structure directly from experimental data without using any prior knowledge or computational input, is extremely rare for 2D-MOFs and COFs. In contrast to SCXRD, three-dimensional electron diffraction (3DED) only requires crystals sized in tens or hundreds of nanometers, making it an ideal method for single-crystal analysis of 2D-MOFs and COFs and obtaining their fine structural details.In this Account, we describe our recent development of the 3DED method and its application in structure determination and property studies of 2D-MOFs and COFs. A key development is the establishment of a continuous 3DED data collection protocol. By collecting electron diffraction (ED) patterns continuously while performing crystal tilting, the electron dose applied to the target nanocrystal is greatly reduced. This allows the acquisition of high-resolution 3DED data from 2D-MOFs and COFs by minimizing their damage under the electron beam. We have also developed an approach to couple 3DED with real-space structure solution methods, i.e., simulated annealing (SA), for single-crystal structural analysis of materials that do not have high crystallinity. We successfully determined two 2D-COF structures by combining 3DED with SA.We provide several examples demonstrating the application of 3DED for the ab initio structure determination of 2D-MOFs and COFs, revealing not only their in-plane structures but also their stacking modes at the atomic level. Notably, the obtained structural details serve as the foundation for further understanding the properties of 2D-MOFs and COFs, such as their electronic band structures, charge mobilities, etc. Beyond structure determination, we describe our work on using 3DED as a high-throughput method for the discovery of new materials. Using this approach, we discovered a novel MOF that was present only in trace amounts within a multiphasic mixture. Through this discovery, we were able to tune the synthesis conditions to obtain its pure phase.We detail how 3DED can be used to probe different levels of molecular motions in MOFs through the analysis of anisotropic displacement parameters (ADPs). Additionally, we show that 3DED can provide accurate information about intermolecular weak interactions such as hydrogen bonding and van der Waals (vdW) interactions. Our studies demonstrate that 3DED is a valuable method for the structural analysis of 2D-MOFs and COFs. We envision that 3DED can accelerate research in these fields by providing unambiguous structural models at the atomic level.

4.
Adv Mater ; 36(38): e2408094, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-39096074

RESUMEN

Multinuclear metal clusters are ideal candidates to catalyze small molecule activation reactions involving the transfer of multiple electrons. However, synthesizing active metal clusters is a big challenge. Herein, on constructing an unparalleled Co4(SO4)4 cluster within porphyrin-based metal-organic frameworks (MOFs) and the electrocatalytic features of such Co4(SO4)4 clusters for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is reported. The reaction of CoII sulfate and metal complexes of tetrakis(4-pyridyl)porphyrin under solvothermal conditions afforded Co4-M-MOFs (M═Co, Cu, and Zn). Crystallographic studies revealed that these Co4-M-MOFs have the same framework structure, having the Co4(SO4)4 clusters connected by metalloporphyrin units through Co─Npyridyl bonds. In the Co4(SO4)4 cluster, the four CoII ions are chemically and symmetrically equivalent and are each coordinated with four sulfate O atoms to give a distorted cube-like structure. Electrocatalytic studies showed that these Co4-M-MOFs are all active for electrocatalytic OER and ORR. Importantly, by regulating the activity of the metalloporphyrin units, it is confirmed that the Co4(SO4)4 cluster is active for oxygen electrocatalysis. With the use of Co porphyrins as connecting units, Co4-Co-MOF displays the highest electrocatalytic activity in this series of MOFs by showing a 10 mA cm-2 OER current density at 357 mV overpotential and an ORR half-wave potential at 0.83 V versus reversible hydrogen electrode (RHE). Theoretical studies revealed the synergistic effect of two proximal Co atoms in the Co4(SO4)4 cluster in OER by facilitating the formation of O─O bonds. This work is of fundamental significance to present the construction of Co4(SO4)4 clusters in framework structures for oxygen electrocatalysis and to demonstrate the cooperation between two proximal Co atoms in such clusters during the O─O bond formation process.

5.
J Am Chem Soc ; 146(36): 25016-25027, 2024 Sep 11.
Artículo en Inglés | MEDLINE | ID: mdl-39213506

RESUMEN

Developing the topochemical polymerization of metal-organic frameworks (MOFs) is of pronounced significance for expanding their functionalities but is still a challenge on third-order nonlinear optics (NLO). Here, we report diacetylene MOF (CAS-1-3) films prepared using a stepwise deposition method and film structural transformation approach, featuring dynamic structural diversity. The MOF structures were determined by the three-dimensional electron diffraction (3D ED) method from nanocrystals collected from the films, which provides a reliable strategy for determining the precise structure of unknown MOF films. We demonstrate the well-aligned diacetylene groups in the MOFs can promote topological polymerization to produce a highly conjugated system under thermal stimulation. As a result, the three MOF films have distinct NLO properties: the CAS-1 film exhibits saturable absorption (SA) while CAS-2 and CAS-3 films exhibit reverse saturable absorption (RSA). Interestingly, due to the topochemical polymerization of the MOF films, a transition from SA to RSA response was observed with increasing temperatures, and the optical limiting effect was significantly enhanced (∼46 times). This study provides a new strategy for preparing NLO materials and thermally regulation of nonlinear optics.

6.
Nano Lett ; 24(25): 7616-7622, 2024 Jun 26.
Artículo en Inglés | MEDLINE | ID: mdl-38815153

RESUMEN

Engineering the building blocks in metal-organic materials is an effective strategy for tuning their dynamical properties and can affect their response to external guest molecules. Tailoring the interaction and diffusion of molecules into these structures is highly important, particularly for applications related to gas separation. Herein, we report a vanadium-based hybrid ultramicroporous material, VOFFIVE-1-Ni, with temperature-dependent dynamical properties and a strong affinity to effectively capture and separate carbon dioxide (CO2) from methane (CH4). VOFFIVE-1-Ni exhibits a CO2 uptake of 12.08 wt % (2.75 mmol g-1), a negligible CH4 uptake at 293 K (0.5 bar), and an excellent CO2-over-CH4 uptake ratio of 2280, far exceeding that of similar materials. The material also exhibits a favorable CO2 enthalpy of adsorption below -50 kJ mol-1, as well as fast CO2 adsorption rates (90% uptake reached within 20 s) that render the hydrolytically stable VOFFIVE-1-Ni a promising sorbent for applications such as biogas upgrading.

7.
ACS Appl Mater Interfaces ; 16(14): 17812-17820, 2024 Apr 10.
Artículo en Inglés | MEDLINE | ID: mdl-38557002

RESUMEN

Two-dimensional metal-organic nanosheets (MONs) have emerged as attractive alternatives to their three-dimensional metal-organic framework (MOF) counterparts for heterogeneous catalysis due to their greater external surface areas and higher accessibility of catalytically active sites. Zr MONs are particularly prized because of their chemical stability and high Lewis and Brønsted acidities of the Zr clusters. Herein, we show that careful control over modulated self-assembly and exfoliation conditions allows the isolation of the first example of a two-dimensional nanosheet wherein Zr6 clusters are linked by dicarboxylate ligands. The hxl topology MOF, termed GUF-14 (GUF = Glasgow University Framework), can be exfoliated into monolayer thickness hns topology MONs, and acid-induced removal of capping modulator units yields MONs with enhanced catalytic activity toward the formation of imines and the hydrolysis of an organophosphate nerve agent mimic. The discovery of GUF-14 serves as a valuable example of the undiscovered MOF/MON structural diversity extant in established metal-ligand systems that can be accessed by harnessing the power of modulated self-assembly protocols.

8.
Microorganisms ; 12(3)2024 Mar 07.
Artículo en Inglés | MEDLINE | ID: mdl-38543590

RESUMEN

Astragalus is a medicinal plant with obvious rhizosphere effects. At present, there are many Astragalus plants with high application value but low recognition and resource reserves in the northwestern area of Yunnan province, China. In this study, metagenomics was used to analyze the microbial diversity and community structure of rhizosphere soil of A. forrestii, A. acaulis, and A. ernestii plants grown in a special high-cold environment of northwestern Yunnan, China, at different altitudes ranging from 3225 to 4353 m. These microbes were taxonomically annotated to obtain 24 phyla and 501 genera for A. forrestii, 30 phyla and 504 genera for A. acaulis, as well as 39 phyla and 533 genera for A. ernestii. Overall, the dominant bacterial phyla included Proteobacteria, Actinobacteria, and Acidobacteria, while the dominant fungal ones were Ascomycota and Basidiomycota. At the genus level, Bradyrhizobium, Afipia, and Paraburkholderia were the most prevalent bacteria, and Hyaloscypha, Pseudogymnoascus, and Russula were the dominant fungal genera. Some of them are considered biocontrol microbes that could sustain the growth and health of host Astragalus plants. Redundancy analysis revealed that pH, TN, and SOM had a significant impact on the microbial community structures (p < 0.05). Finally, triterpene, flavonoid, polysaccharide, and amino acid metabolisms accounted for a high proportion of the enriched KEGG pathways, which possibly contributed to the synthesis of bioactive constituents in the Astragalus plants.

9.
Chem Sci ; 14(43): 12056-12067, 2023 Nov 08.
Artículo en Inglés | MEDLINE | ID: mdl-37969597

RESUMEN

3D-oriented metal-organic framework (MOF) films and patterns have recently emerged as promising platforms for sensing and photonic applications. These oriented polycrystalline materials are typically prepared by heteroepitaxial growth from aligned inorganic nanostructures and display anisotropic functional properties, such as guest molecule alignment and polarized fluorescence. However, to identify suitable conditions for the integration of these 3D-oriented MOF superstructures into functional devices, the effect of water (gaseous and liquid) on different frameworks should be determined. We note that the hydrolytic stability of these heteroepitaxially grown MOF films is currently unexplored. In this work, we present an in-depth analysis of the structural evolution of aligned 2D and 3D Cu-based MOFs grown from Cu(OH)2 coatings. Specifically, 3D-oriented Cu2L2 and Cu2L2DABCO films (L = 1,4-benzenedicarboxylate, BDC; biphenyl-4,4-dicarboxylate, BPDC; DABCO = 1,4-diazabicyclo[2.2.2]octane) were exposed to 50% relative humidity (RH), 80% RH and liquid water. The combined use of X-ray diffraction, infrared spectroscopy, and scanning electron microscopy shows that the sensitivity towards humid environments critically depends on the presence of the DABCO pillar ligand. While oriented films of 2D MOF layers stay intact upon exposure to all levels of humidity, hydrolysis of Cu2L2DABCO is observed. In addition, we report that in environments with high water content, 3D-oriented Cu2(BDC)2DABCO recrystallizes as 3D-oriented Cu2(BDC)2. The heteroepitaxial MOF-to-MOF transformation mechanism was studied with in situ synchrotron experiments, time-resolved AFM measurements, and electron diffraction. These findings provide valuable information on the stability of oriented MOF films for their application in functional devices and highlight the potential for the fabrication of 3D-oriented superstructures via MOF-to-MOF transformations.

10.
J Am Chem Soc ; 145(43): 23630-23638, 2023 Nov 01.
Artículo en Inglés | MEDLINE | ID: mdl-37852932

RESUMEN

Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have emerged as a new class of crystalline layered conducting materials that hold significant promise for applications in electronics and spintronics. However, current 2D c-MOFs are mainly made from organic planar ligands, whereas layered 2D c-MOFs constructed by curved or twisted ligands featuring novel orbital structures and electronic states remain less developed. Herein, we report a Cu-catecholate wavy 2D c-MOF (Cu3(HFcHBC)2) based on a fluorinated core-twisted contorted hexahydroxy-hexa-cata-hexabenzocoronene (HFcHBC) ligand. We show that the resulting film is composed of rod-like single crystals with lengths up to ∼4 µm. The crystal structure is resolved by high-resolution transmission electron microscopy (HRTEM) and continuous rotation electron diffraction (cRED), indicating a wavy honeycomb lattice with AA-eclipsed stacking. Cu3(HFcHBC)2 is predicted to be metallic based on theoretical calculation, while the crystalline film sample with numerous grain boundaries apparently exhibits semiconducting behavior at the macroscopic scale, characterized by obvious thermally activated conductivity. Temperature-dependent electrical conductivity measurements on the isolated single-crystal devices indeed demonstrate the metallic nature of Cu3(HFcHBC)2, with a very weak thermally activated transport behavior and a room-temperature conductivity of 5.2 S cm-1. Furthermore, the 2D c-MOFs can be utilized as potential electrode materials for energy storage, which display decent capacity (163.3 F g-1) and excellent cyclability in an aqueous 5 M LiCl electrolyte. Our work demonstrates that wavy 2D c-MOF using contorted ligands are capable of intrinsic metallic transport, marking the emergence of new conductive MOFs for electronic and energy applications.

11.
Commun Chem ; 6(1): 116, 2023 Jun 07.
Artículo en Inglés | MEDLINE | ID: mdl-37286771

RESUMEN

Covalent organic frameworks (COFs) have been attracting intense research due to their permanent porosity, designable architecture, and high stability. However, COFs are challenging to crystallize and their synthesis often results in tiny crystal sizes and low crystallinities, which hinders an unambiguous structure determination. Herein, we demonstrate that the structure of low-crystallinity COF Py-1P nanocrystals can be solved by coupling three-dimensional electron diffraction (3DED) with simulated annealing (SA). The resulting model is comparable to that obtained from high-crystallinity samples by dual-space method. Moreover, for low-resolution 3DED data, the model obtained by SA shows a better framework than those provided by classic direct method, dual-space method, and charge flipping. We further simulate data with different resolutions to understand the reliability of SA under different crystal quality conditions. The successful determination of Py-1P structure by SA compared to other methods provides new knowledge for using 3DED to analyze low-crystallinity and nanosized materials.

12.
ACS Appl Mater Interfaces ; 15(14): 17938-17946, 2023 Apr 12.
Artículo en Inglés | MEDLINE | ID: mdl-37009862

RESUMEN

Owing to the capacity boost from anion redox activities, cation-disordered rock-salt oxides are considered as potential candidates for the next-generation of high energy density Li-ion cathode materials. Unfortunately, the anion redox process that affords ultra-high specific capacity often triggers irreversible O2 release, which brings about structural degradation and rapid capacity decay. In this study, we present a partial chlorine (Cl) substitution strategy to synthesize a new cation-disordered rock-salt compound of Li1.225Ti0.45Mn0.325O1.9Cl0.1 and investigate the impact of Cl substitution on the oxygen redox process and the structural stability of cation-disordered rock-salt cathodes. We find that partial replacement of O2- by Cl- expands the cell volume and promotes anion redox reaction reversibility, thus increasing the Li+ ion diffusion rate and suppressing irreversible lattice oxygen loss. As a result, the Li1.225Ti0.45Mn0.325O1.9Cl0.1 cathode exhibits significantly improved cycling durability at high current densities, compared with the pristine Li1.225Ti0.45Mn0.325O2 cathode. This work demonstrates the promising feasibility of the Cl substitution process for advanced cation-disordered rock-salt cathode materials.

13.
Angew Chem Int Ed Engl ; 62(25): e202300186, 2023 Jun 19.
Artículo en Inglés | MEDLINE | ID: mdl-36862366

RESUMEN

Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) are emerging as a unique class of electronic materials. However, 2D c-MOFs with band gaps in the Vis-NIR and high charge carrier mobility are rare. Most of the reported conducting 2D c-MOFs are metallic (i.e. gapless), which largely limits their use in logic devices. Herein, we design a phenanthrotriphenylene-based, D2h -symmetric π-extended ligand (OHPTP), and synthesize the first rhombic 2D c-MOF single crystals (Cu2 (OHPTP)). The continuous rotation electron diffraction (cRED) analysis unveils the orthorhombic crystal structure at the atomic level with a unique slipped AA stacking. The Cu2 (OHPTP) is a p-type semiconductor with an indirect band gap of ≈0.50 eV and exhibits high electrical conductivity of 0.10 S cm-1 and high charge carrier mobility of ≈10.0 cm2  V-1 s-1 . Theoretical calculations underline the predominant role of the out-of-plane charge transport in this semiquinone-based 2D c-MOF.


Asunto(s)
Estructuras Metalorgánicas , Conductividad Eléctrica , Electrónica , Electrones , Cetonas
14.
Oncol Lett ; 25(3): 116, 2023 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-36844615

RESUMEN

How to efficiently obtain high-purity cancer stem cells (CSCs) has been the basis of CSC research, but the optimal conditions for serum-free suspension culture of CSCs are still unclear. The present study aimed to define the optimal culture medium composition and culture time for the enrichment of colon CSCs via suspension culture. Suspension cell cultures of colon cancer DLD-1 cells were prepared using serum-free medium (SFM) containing variable concentrations of epidermal growth factor (EGF) and basic fibroblast growth factor (bFGF) to produce spheroids. Culture times were set at 10, 20 and 30 days. A total of nine different concentrations of EGF and bFGF were added to SFM to generate nine experimental groups. The proportions of CD44+, CD133+, and CD44+CD133+ double-positive spheroid cells were detected via flow cytometry. mRNA expression of stemness-, epithelial-mesenchymal transition- and Wnt/ß-catenin pathway-associated genes was determined via reverse transcription-quantitative PCR. Self-renewal ability was evaluated by a sphere-forming assay. Tumorigenesis was studied in vitro using a colony formation assay and in vivo via subcutaneous cell injection in nude mice. It was found that the highest expression proportions of CD133+ and CD44+ spheroid cells were observed in group (G)9 (20 ng/ml EGF + 20 ng/ml bFGF) at 30 days (F=123.554 and 99.528, respectively, P<0.001), CD133+CD44+ cells were also observed in G9 at 30 days (and at 10 days in G3 and 20 days in G6; F=57.897, P<0.001). G9 at 30 days also displayed the highest expression of Krüppel-like factor 4, leucine-rich repeat-containing G protein-coupled receptor 5, CD44, CD133, Vimentin and Wnt-3a (F=22.682, 25.401, 3.272, 7.852, 13.331 and 17.445, respectively, P<0.001) and the lowest expression of E-cadherin (F=10.851, P<0.001). G9 at 30 days produced the highest yield of cell spheroids, as determined by a sphere forming assay (F=19.147, P<0.001); colony formation assays also exhibited the greatest number of colonies derived from G9 spheroids at 30 days (F=60.767, P<0.01), which also generated the largest mean tumor volume in the subcutaneous tumorigenesis xenograft model (F=12.539, P<0.01). In conclusion, 20 ng/ml EGF + 20 ng/ml bFGF effectively enriched colon CSCs when added to suspension culture for 30 days, and conferred the highest efficiency compared with other combinations.

15.
Anal Bioanal Chem ; 415(6): 1173-1185, 2023 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-36607393

RESUMEN

Proteins, and more specifically glycoproteins, have been widely used as biomarkers, e.g., to monitor disease states. Bottom-up approaches based on mass spectrometry (MS) are techniques commonly utilized in glycoproteomics, involving protein digestion and glycopeptide enrichment. Here, a dual function polymeric thiol-ene-based microfluidic chip (TE microchip) was applied for the analysis of the proteins osteopontin (OPN) and immunoglobulin G (IgG), which have important roles in autoimmune diseases, in inflammatory diseases, and in coronavirus disease 2019 (COVID-19). TE microchips with larger internal surface features immobilized with trypsin were successfully utilized for OPN digestion, providing rapid and efficient digestion with a residence time of a few seconds. Furthermore, TE microchips surface-modified with ascorbic acid linker (TEA microchip) have been successfully utilized for IgG glycopeptide enrichment. To illustrate the use of the chips for more complex samples, they were applied to enrich IgG glycopeptides from human serum samples with antibodies against severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). The dual functional TE microchips could provide high throughput for online protein digestion and glycopeptide enrichment, showing great promise for future extended applications in proteomics and the study of related diseases.


Asunto(s)
COVID-19 , Glicopéptidos , Humanos , Glicopéptidos/química , Inmunoglobulina G , Osteopontina , Compuestos de Sulfhidrilo , Microfluídica , SARS-CoV-2 , Inflamación , Digestión
16.
Nanomaterials (Basel) ; 12(18)2022 Sep 10.
Artículo en Inglés | MEDLINE | ID: mdl-36144929

RESUMEN

Zero-dimensional (0D) hybrid manganese halides have emerged as promising platforms for the white light-emitting diodes (w-LEDs) owing to their excellent optical properties. Necessary for researching on the structure-activity relationship of photoluminescence (PL), the novel manganese bromides (C13H14N)2MnBr4 and (C13H26N)2MnBr4 are reported by screening two ligands with similar atomic arrangements but various steric configurations. It is found that (C13H14N)2MnBr4 with planar configuration tends to promote a stronger electron-phonon coupling, crystal filed effect and concentration-quenching effect than (C13H26N)2MnBr4 with chair configuration, resulting in the broadband emission (FWHM = 63 nm) to peak at 539 nm with a large Stokes shift (70 nm) and a relatively low photoluminescence quantum yield (PLQY) (46.23%), which makes for the potential application (LED-1, Ra = 82.1) in solid-state lighting. In contrast, (C13H26N)2MnBr4 exhibits a narrowband emission (FWHM = 44 nm) which peaked at 515 nm with a small Stokes shift (47 nm) and a high PLQY of 64.60%, and the as-fabricated white LED-2 reaches a wide colour gamut of 107.8% National Television Standards Committee (NTSC), thus highlighting the immeasurable application prospects in solid-state display. This work clarifies the significance of the spatial configuration of organic cations in hybrids perovskites and enriches the design ideas for function-oriented low-dimensional emitters.

17.
ACS Appl Mater Interfaces ; 14(34): 38865-38874, 2022 Aug 31.
Artículo en Inglés | MEDLINE | ID: mdl-35960601

RESUMEN

Cation-disordered rock-salt cathode materials are featured by their extraordinarily high specific capacities in lithium-ion batteries primarily contributed by anion redox reactions. Unfortunately, anion redox reactions can trigger oxygen release in this class of materials, leading to fast capacity fading and major safety concern. Despite the capability of absorbing structural distortions, high-ratio d0 transition-metal cations are considered to be unfavorable in design of a new cation-disordered rock-salt structure because of their electrochemically inactive nature. Herein, we report a new cation-disordered rock-salt compound of Li1.2Ti0.6Mn0.2O2 with the stoichiometry of Ti4+ as high as 0.6. The capacity reducing effect by the low-ratio active transition-metal center can be balanced by using a Mn2+/Mn4+ two-electron redox couple. The strengthened networks of strong Ti-O bonds greatly retard the oxygen release and improve the structural stability of cation-disordered rock-salt cathode materials. As expected, Li1.2Ti0.6Mn0.2O2 delivers significantly improved electrochemical performances and thermal stability compared to the low-ratio Ti4+ counterpart of Li1.2Ti0.4Mn0.4O2. Theoretical simulations further reveal that the improved electrochemical performances of Li1.2Ti0.6Mn0.2O2 are attributed to its lower Li+ diffusion energy barrier and enhanced unhybridized O 2p states compared to Li1.2Ti0.4Mn0.4O2. This concept might be helpful for the improvement of structural stability and electrochemical performances of other cation-disordered rock-salt metal oxide cathode materials.

18.
Burns ; 48(3): 633-638, 2022 05.
Artículo en Inglés | MEDLINE | ID: mdl-34272079

RESUMEN

BACKGROUND: The aim of this study was to explore expression levels and clinical values of miR-21 and miR-210 in patients with sepsis after burns. METHODS: One hundred and twenty-eight burn patients who were treated in Binzhou Medical University Hospital were selected as research objects, among which 69 complicated with sepsis were in an observation group and 59 complicated with infection were in a control group. MiR-21 and miR-210 expression in the patients' serum was detected by RT-PCR. Serum inflammatory cytokines were detected by an enzyme-linked immunosorbent assay (ELISA). Correlation analysis was used for the correlations of the miR-21 and miR-210 with the cytokines. Receiver operating characteristic (ROC) curves were plotted to analyze the diagnostic values of the miR-21 and miR-210 for sepsis after burns and their predictive values for the poor prognosis of sepsis patients. RESULTS: MiR-21 expression reduced remarkably and miR-210 expression rose remarkably in the serum of patients with sepsis after burns. According to the analysis of the ROC curves, both of the miR-21 and miR-210 had relatively high diagnostic sensitivity for the disease, but the diagnostic value of their combined detection was higher. Contents of hs-CRP, TNF-α, IL-6, and ICAM-1 in serum were remarkably higher in the observation group than those in the control group. According to the correlation analysis, miR-21 was negatively correlated with the expression of the four cytokines, while miR-210 was positively correlated with that. The predictive value of miR-21 for the prognosis of sepsis patients was not high, but miR-210 had a certain predictive value, and their combined detection had a higher value. CONCLUSION: In serum of patients with sepsis after burns, miR-21 expression reduces remarkably and miR-210 expression rises. The miR-21 and miR-210 are related to the degree of inflammatory responses in septic patients, and their combined detection has a certain value for diagnosing the disease and predicting its prognosis.


Asunto(s)
Quemaduras , MicroARNs , Sepsis , Quemaduras/complicaciones , Proteína C-Reactiva , Citocinas , Humanos , Molécula 1 de Adhesión Intercelular , Interleucina-6 , Pronóstico , Curva ROC , Factor de Necrosis Tumoral alfa
19.
Front Microbiol ; 12: 729744, 2021.
Artículo en Inglés | MEDLINE | ID: mdl-34659157

RESUMEN

Objective: This work was conducted in order to study the effect of the lower genital tract (vaginal and cervical canal) microbiota on pregnancy outcomes of reproductive-aged women receiving embryo transfer. Study design: A total of 150 reproductive-aged patients who received the first fresh in vitro fertilization-embryo transfer (IVF-ET) were included in the study. Samples from the vagina and cervical site of each patient were collected separately using sterile swabs before ET. Genomic DNA was pyrosequenced for the V3-V4 regions of the 16S ribosomal RNA gene. Further bioinformatics analysis was performed using QIIME and R package. Pregnancy outcomes were followed and analyzed to compare differences in microbial composition. Results: The cervical microbiota had a higher Shannon index than the vaginal microbiota, and the microbial composition was different between the two sites. However, the Sorenson index between the two sites within the same individual was 0.370 (0.309-0.400). A total of 89 patients achieved clinical pregnancy after ET, while 61 failed. The Shannon indices and the microbial community of both vaginal and cervical microbiota between pregnant and non-pregnant groups were not significantly different. The relative abundance of Lactobacillus in the vagina and cervical canal did not differ between the two groups. Linear discriminant analysis, random forest analysis, and receiver-operating characteristic curve analysis showed that Bifidobacterium, Prevotella, and Lactobacillus iners in the vagina, as well as Solanum torvum, Fusobacterium, and Streptococcus in the cervix, may be negatively associated with clinical pregnancy after IVF. Conclusion: The cervical microbiota was more diverse than the vaginal microbiota, but because of anatomical continuity, there was a correlation between the two sites. The microbial composition of the vagina and cervical canal may influence the outcome of IVF-ET, but more samples are needed to verify this conclusion.

SELECCIÓN DE REFERENCIAS
DETALLE DE LA BÚSQUEDA