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1.
Commun Biol ; 7(1): 715, 2024 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-38858498

RESUMO

In cryo-electron microscopy (cryo-EM), sample preparation poses a critical bottleneck, particularly for rare or fragile macromolecular assemblies and those suffering from denaturation and particle orientation distribution issues related to air-water interface. In this study, we develop and characterize an immobilized antibody-based affinity grid (IAAG) strategy based on the high-affinity PA tag/NZ-1 antibody epitope tag system. We employ Pyr-NHS as a linker to immobilize NZ-1 Fab on the graphene oxide or carbon-covered grid surface. Our results demonstrate that the IAAG grid effectively enriches PA-tagged target proteins and overcomes preferred orientation issues. Furthermore, we demonstrate the utility of our IAAG strategy for on-grid purification of low-abundance target complexes from cell lysates, enabling atomic resolution cryo-EM. This approach greatly streamlines the purification process, reduces the need for large quantities of biological samples, and addresses common challenges encountered in cryo-EM sample preparation. Collectively, our IAAG strategy provides an efficient and robust means for combined sample purification and vitrification, feasible for high-resolution cryo-EM. This approach holds potential for broader applicability in both cryo-EM and cryo-electron tomography (cryo-ET).


Assuntos
Anticorpos Imobilizados , Microscopia Crioeletrônica , Microscopia Crioeletrônica/métodos , Anticorpos Imobilizados/química , Anticorpos Imobilizados/imunologia , Grafite/química , Humanos
2.
J Am Chem Soc ; 146(12): 8352-8361, 2024 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-38494762

RESUMO

Highly Li-concentrated electrolytes have been widely studied to harness their uniquely varying bulk and interface properties that arise from their distinctive physicochemical properties and coordination structures. Similar strategies have been applied in the realm of ionic liquid electrolytes to exploit their improved functionalities. Despite these prospects, the impact of organic cation behavior on interfacial processes remains largely underexplored compared to the widely studied anion behavior. The present study demonstrates that the weakened interactions between cations and anions engender "unprotected" organic cations in highly Li-concentrated ionic liquid electrolytes, leading to the decomposition of electrolytes during the initial charge. This decomposition behavior is manifested by the substantial irreversible capacities and inferior initial Coulombic efficiencies observed during the initial charging of graphite negative electrodes, resulting in considerable electrolyte consumption and diminished energy densities in full-cell configurations. The innate cation behavior is ascertained by examining the coordination environment of ionic liquid electrolytes with varied Li concentrations, where intricate ionic interactions between organic cations and anions are unveiled. In addition, anionic species with high Lewis basicity were introduced to reinforce the ionic interactions involving organic cations and improve the initial Coulombic efficiency. This study verifies the role of unprotected organic cations while highlighting the significance of the coordination environment in the performance of ionic liquid electrolytes.

4.
Sensors (Basel) ; 23(7)2023 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-37050758

RESUMO

The localization of sensor nodes is an important problem in wireless sensor networks. The DV-Hop algorithm is a typical range-free algorithm, but the localization accuracy is not high. To further improve the localization accuracy, this paper designs a DV-Hop algorithm based on multi-objective salp swarm optimization. Firstly, hop counts in the DV-Hop algorithm are subdivided, and the average hop distance is corrected based on the minimum mean-square error criterion and weighting. Secondly, the traditional single-objective optimization model is transformed into a multi-objective optimization model. Then, in the third stage of DV-Hop, the improved multi-objective salp swarm algorithm is used to estimate the node coordinates. Finally, the proposed algorithm is compared with three improved DV-Hop algorithms in two topologies. Compared with DV-Hop, The localization errors of the proposed algorithm are reduced by 50.79% and 56.79% in the two topology environments with different communication radii. The localization errors of different node numbers are decreased by 38.27% and 56.79%. The maximum reductions in localization errors are 38.44% and 56.79% for different anchor node numbers. Based on different regions, the maximum reductions in localization errors are 56.75% and 56.79%. The simulation results show that the accuracy of the proposed algorithm is better than that of DV-Hop, GWO-DV-Hop, SSA-DV-Hop, and ISSA-DV-Hop algorithms.

5.
ACS Appl Mater Interfaces ; 15(13): 16865-16873, 2023 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-36946616

RESUMO

A flexible humidity sensor with wide sensing range, superior sensitivity, high linearity, and advanced response/recovery capabilities is extremely desirable for practical applications in human body-related (HBR) monitoring and human-machine interaction (HMI). However, the practical sensor lacks a versatile nanomaterial integrated with sensing capabilities and mechanical flexibility to meet the criteria. Herein, a comprehensive flexible humidity sensor with ultralong Na2Ti3O7 nanowires (>120 µm) is subtly constructed for the first time. Owing to the distinguish nanowires network structure, the sensor exhibits wide sensing range (11-95% RH), high sensitivity (>103), high linearity (R2 > 0.98), and fast response/recovery capability (8.9/2.1 s), as well as excellent respiratory stability (>5000 s). In addition, the Na2Ti3O7-based humidity sensor demonstrates superior flexibility and antibacteria capabilities, and exhibits diverse applications in respiration monitoring, noncontact detection, as well as dynamic interactive display. This work provides a multifunctional humidity sensor with excellent practicability, suggesting the great potential in next-generation human-related flexible/wearable devices.

6.
ACS Nano ; 17(5): 4862-4870, 2023 03 14.
Artigo em Inglês | MEDLINE | ID: mdl-36825732

RESUMO

Flexible piezosensing electronic skins (e-skins) have attracted considerable interest owing to their applications in real-time human-health monitoring, human-machine interactions, and soft bionic robot perception. However, the fabrication of piezosensing e-skins with high sensitivity, biological affinity, and good permeability at the same time is challenging. Herein, we designed and synthesized Mo2S3 nanowires by inserting ∞1[Mo2+S] chains between MoS2 interlayers. The resulting Mo2S3 nanowires feature high conductivity (4.9 × 104 S m-1) and a high aspect ratio (∼200). An ultrathin (∼500 nm) Mo2S3 nanowire network was fabricated using a simple liquid/liquid interface self-assembly method, showing high piezoresistive sensitivity (5.65 kPa-1), a considerably low pressure detection limit (0.08 Pa), and gratifying air permeability. Moreover, this nanowire network can be directly attached to human skin for real-time human pulse detection, finger movement monitoring, and sign language recognition, exhibiting excellent potential for health monitoring and human-machine interactions.


Assuntos
Nanofios , Robótica , Dispositivos Eletrônicos Vestíveis , Humanos , Pele , Condutividade Elétrica
7.
ChemSusChem ; 16(10): e202202185, 2023 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-36807548

RESUMO

Bamboo is widely distributed, rapidly regenerable, and incorporates long cellulose fibers, which make it one of the most lightweight and strong natural materials. Processing bamboo into a high-performance structural material for plastic replacement is highly promising but challenging. In this study, an all-natural, high-performance structural material is derived from natural bamboo with superior mechanical and thermal properties that benefit from the introduction of surface charge and further layer-by-layer assembly of bamboo cellulose fibers. The obtained modified bamboo fiber plate (MBFP) transcends the constraints of the natural size and anisotropy of bamboo, showing high flexural strength (ca. 179 MPa) and flexural modulus (ca. 12 GPa). Moreover, the product has an extremely low coefficient of thermal expansion (ca. 11.3×10-6  K-1 ), high thermal stability, and superior fire resistance. The excellent mechanical and thermal properties combined with the efficient and rational manufacturing process make MBFP a powerful plastic alternative for furniture, construction, and automotive industries.

8.
ACS Appl Mater Interfaces ; 14(17): 19426-19436, 2022 May 04.
Artigo em Inglês | MEDLINE | ID: mdl-35446016

RESUMO

Niobium pentoxide (Nb2O5) represents an exquisite class of negative electrode materials with unique pseudocapacitive kinetics that engender superior power and energy densities for advanced electrical energy storage devices. Practical energy devices are expected to maintain stable performance under real-world conditions such as temperature fluctuations. However, the intercalation pseudocapacitive behavior of Nb2O5 at elevated temperatures remains unexplored because of the scarcity of suitable electrolytes. Thus, in this study, we investigate the effect of temperature on the pseudocapacitive behavior of submicron-sized Nb2O5 in a wide potential window of 0.01-2.3 V. Furthermore, ex situ X-ray diffraction and X-ray photoelectron spectroscopy reveal the amorphization of Nb2O5 accompanied by the formation of NbO via a conversion reaction during the initial cycle. Subsequent cycles yield enhanced performance attributed to a series of reversible NbV, IV/NbIII redox reactions in the amorphous LixNb2O5 phase. Through cyclic voltammetry and symmetric cell electrochemical impedance spectroscopy, temperature elevation is noted to increase the pseudocapacitive contribution of the Nb2O5 electrode, resulting in a high rate capability of 131 mAh g-1 at 20,000 mA g-1 at 90 °C. The electrode further exhibits long-term cycling over 2000 cycles and high Coulombic efficiency ascribed to the formation of a robust, [FSA]--originated solid-electrolyte interphase during cycling.

9.
Chemistry ; 28(23): e202200124, 2022 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-35170808

RESUMO

Polyvinyl chloride (PVC) is widely used in daily life, but its waste has become a serious environmental problem. A solid base assisted low-temperature solvothermal dehalogenation was developed in this work to sustainably and efficiently transform PVC into high-value dimethylamine hydrochloride (DMACl) chemical and N,O co-doped carbon monolith with hierarchically porous structure. The synergistic promotion of solid-base catalyst and solvent decomposition with the removal of HCl can shift forward the chemical equilibrium to promote the dechlorination of PVC and increase the carbon yield. Meanwhile, the solid-base catalyst can also act as a pore-forming additive to fabricate the carbon monolith with hierarchical pores. Induced by the high specific surface area, hierarchical pores and N,O co-doped structure, the generated carbon monolith exhibits superior electrocatalytic performance towards H2 evolution. These discoveries shed light on the design of synergistically coupled solvent and solid catalyst to promote the heterogeneous conversion of waste chlorinated plastics into high-value chemicals for a sustainable future.

10.
Adv Mater ; 34(9): e2108505, 2022 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-34969159

RESUMO

Alkaline water electrolysis is commercially desirable to realize large-scale hydrogen production. Although nonprecious catalysts exhibit high electrocatalytic activity at low current density (10-50 mA cm-2 ), it is still challenging to achieve industrially required current density over 500 mA cm-2  due to inefficient electron transport and competitive adsorption between hydroxyl and water. Herein, the authors design a novel metallic heterostructure based on nickel nitride and monoclinic molybdenum disulfide (Ni3 N@2M-MoS2 ) for extraordinary water electrolysis. The Ni3 N@2M-MoS2  composite with heterointerface provides two kinds of separated reaction sites to overcome the steric hindrance of competitive hydroxyl/water adsorption. The kinetically decoupled hydroxyl/water adsorption/dissociation and metallic conductivity of Ni3 N@2M-MoS2  enable hydrogen production from Ni3 N and oxygen evolution from the heterointerface at large current density. The metallic heterostructure is proved to be imperative for the stabilization and activation of Ni3 N@2M-MoS2 , which can efficiently regulate the active electronic states of Ni/N atoms around the Fermi-level through the charge transfer between the active atoms of Ni3 N and MoMo bonds of 2M-MoS2  to boost overall water splitting. The Ni3 N@2M-MoS2  incorporated water electrolyzer requires ultralow cell voltage of 1.644 V@1000 mA cm-2  with ≈100% retention over 300 h, far exceeding the commercial Pt/C║RuO2 (2.41 V@1000 mA cm-2 , 100 h, 58.2%).

11.
Chemistry ; 27(8): 2717-2723, 2021 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-33063319

RESUMO

Metal-organic frameworks (MOFs) can become promising electrode materials for advanced lithium-ion batteries (LIBs), because their loosely packed porous structures may mitigate volume expansion and metal atom aggregation, which occur at the respective metal oxides. However, they suffer from poor electrical conductivity and irreversible structural degradation upon charge/discharge processes, which impede their practical utilization. Herein, we investigate MOF-like Sn2 O(CN2 ) as a new electrode material. The conductive yet flexible [N=C=N] linkers are tilted between [Sn4 O] nodes and cross-linked into a porous quasi-layered structure. Such structure offers abundant channels for fast Li-ion transport and tolerance of enormous volume expansion. Notably, anisotropic [N=C=N]2- arrays hardly migrate so that Sn0 nanodots are physically separated via robust [N=C=N]2- framework during discharge, thereby effectively preventing the formation of large Sn islands. Owing to the structural advantage, the Sn2 O(CN2 ) electrode exhibits an initial Coulombic efficiency as high as ∼80 %. With the addition of graphite as conductive supporter, the electrode provides 978 mAh g-1 at 1.0 A g-1 even after 300 cycles. Such MOF-like carbodiimides hold potential for the advanced electrodes in LIBs and other battery systems.

12.
Chem Commun (Camb) ; 56(71): 10289-10292, 2020 Sep 14.
Artigo em Inglês | MEDLINE | ID: mdl-32756688

RESUMO

To work against the volume expansion (∼300%) of SnO2 during lithiation, here a sub-micro sized, interconnected, and porous SnO2 cube with rationally designed reserved space (∼375%) is synthesized via an artful topochemistry route (CaSn(OH)6-CaSnO3-SnO2). Owing to its microstructure, this novel material harvests enhanced lithium-storage performance.

13.
Inorg Chem ; 59(10): 6785-6789, 2020 May 18.
Artigo em Inglês | MEDLINE | ID: mdl-32369350

RESUMO

Chevrel-phase superconducting compounds AyMo6Q8 (A = Pb, Mg, etc. and Q = S, Se, Te) have attracted much attention due to their ultrahigh upper critical magnetic fields (Hc2). However, the binary compounds Mo6S8 and Mo6Te8 show no superconducting properties above 2 K. In this work, the new Chevrel-phase pseudobinary compound Mo6S6.8Te1.2 with a superconducting transition temperature (Tc) of 3.6 K was successfully synthesized by a two-step process. A detailed investigation implies that the superconductivity in Mo6S6.8Te1.2 may derive from the increased electronic density near the Fermi level in comparison to Mo6S8. Our work provides a feasible scheme to search for new superconducting compounds.

14.
Nanoscale ; 12(10): 6089-6095, 2020 Mar 12.
Artigo em Inglês | MEDLINE | ID: mdl-32129400

RESUMO

Highly active bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) play a pivotal role in Zn-air batteries. The high cost, scarcity and instability of precious-metal-based electrocatalysts for the ORR and OER dramatically hamper their practical application in such clean-energy set-ups. Here, we report highly active Co5.47N-loaded N-doped carbon (CoNMC), prepared via the direct NH3 annealing of a millet-CoCl2 mixture, which is a cheap and mass-producible form of biomass. The optimized product shows superior ORR activity (a half-wave potential of 0.81 V vs. RHE) and electrochemical stability (a 16.5 mV negative shift of the half-wave potential after 2000 cycles) in alkaline media. Also, it shows appealing OER activity (an operating potential at 10 mA cm-2 of 1.62 V vs. RHE). This excellent electrochemical performance can be attributed to the formation of active Co5.47N nanoparticles, the large specific surface area, the abundance of nitrogen active sites, and the high graphitization degree. When assembled into a Zn-air battery, the CoNMC-based cell shows comparable performance to a Pt/C-RuO2 one.

15.
Small ; 16(5): e1905328, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31922697

RESUMO

Exploring the origin of transition metal (TM) lattice-doped layered double hydroxides (LDHs) toward the oxygen evolution reaction (OER) plays a crucial role in engineering efficient electrocatalysts. Without understanding the physics behind the TM-induced catalytic enhancements, it would be challenging to design the next generation of electrocatalysts. Herein, single Ru atoms are introduced into a CoCr LDHs lattice to improve activity. In 0.1 m KOH, CoCrRu LDHs require only 290 mV overpotential to drive to 10 mA cm-2 and show a Tafel slope of 56.12 mV dec-1 . Electronic structure analyses based on density functional theory confirm that promoted OER activity originates from synergetic charge transfer among Ru, Cr, and Co elements. Specifically, Ru dopants can downshift d states of Co and enhance electron donation of Cr to oxygenates, which essentially breaks the scaling relation and achieves higher activity. This work provides insights into how single atomic Ru dopant tunes the electronic structures of its neighbor's active site Co and thus increases OER activities.

16.
Int J Biol Macromol ; 141: 150-160, 2019 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-31487514

RESUMO

Three polysaccharides (WZP1, WZP2, WZP3) and their Se-enriched products (SeWZP1, SeWZP2 and SeWZP3) were obtained from Pleurotus ostreatus using a simple, rapid method and HNO3-Na2SeO3 method, respectively. The molecular weight distribution profiles of all samples except SeWZP2 showed double peaks. The average molecular weights (Mw) of WZP1-3 were 48.6 kDa, 20.2 kDa and 11.8 kDa, respectively, and of SeWZP1-3 were 19.6 kDa, 37.7 kDa, 14.5 kDa, respectively. The complexity of monosaccharide composition of WZP1-3 was inversely proportional to the ethanol concentration used in the ethanol precipitation process. Additionally, the results of biological activity tests indicated that α-glucosidase inhibitory activity of WZP1-3 was related to the molecular weight and the monosaccharide composition complexity. The selenized modification can improve the α-glucosidase-inhibiting, hydroxyl radical-scavenging activity of P. ostreatus polysaccharides. Therefore, by improving their bioactivities by selenization, the polysaccharides of P. ostreatus could be utilized as a natural health food supplement.


Assuntos
Sequestradores de Radicais Livres/química , Polissacarídeos Fúngicos/química , Inibidores de Glicosídeo Hidrolases/química , Pleurotus/química , Peso Molecular , Ácido Nítrico/química , Selenito de Sódio/química
17.
Molecules ; 24(12)2019 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-31207987

RESUMO

Starches from the bulbils of Dioscoreae opposita Thunb. cv. Tiegun were isolated by aqueous steeping (SBS), enzyme extraction (EBS), and alkaline extraction (ABS) methods, respectively. The physicochemical, mineral composition, thermal and morphological characteristics of these starches were investigated. The starch granules were oval, spherical and kidney-shaped and its crystal type is a mixture of A-type and B-type patterns. The starches having larger average granule size showed more amylose and phosphorus contents than those with smaller average granule size. Differential scanning calorimetry (DSC) showed that the SBS had an endothermic transition ranging from 65.8 °C to 76.3 °C with an enthalpy of 2.0 J/g. The endothermic transitions of ABS and EBS showed the regions of 67.9 °C to 73.0 °C, and 66.8 °C to 82.0 °C, respectively. The gelationization enthalpies of ABS and EBS were 13.8 and 11.5 J/g, respectively. Additionally, ABS presented greater clarity in comparison with EBS and SBS. Pasting properties indicated that ABS had the highest peak viscosity, breakdown, but SBS had the lowest trough, final viscosity, setback, and pasting temperature. Generally, ABS and EBS could be used as food thickener or frozen food additives. SBS and EBS were potential technological alternatives in quality preservation of frozen starch-based products and other industrial applications.


Assuntos
Dioscorea/química , Compostos Fitoquímicos/química , Compostos Fitoquímicos/isolamento & purificação , Amido/química , Amido/isolamento & purificação , Solubilidade , Espectroscopia de Infravermelho com Transformada de Fourier , Amido/ultraestrutura , Termodinâmica , Difração de Raios X
18.
Bioorg Med Chem Lett ; 22(2): 806-10, 2012 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-22217877

RESUMO

Two series of novel Dasatinib derivatives have been designed and synthesized, with their in vitro cytostatic effect screened on human chronic myeloid leukemia cell line K562 and human myeloid leukemia cell line U937. Some target compounds demonstrated significant inhibitory activities against both cell lines. Compared to the contrast drug Dasatinib, 1b, 1c, 1d, 1e and 1f were found to demonstrate more potent antitumor activities. The structures of all the newly synthesized compounds were determined by (1)H NMR and (13)C NMR.


Assuntos
Antineoplásicos/síntese química , Antineoplásicos/farmacologia , Desenho de Fármacos , Pirimidinas/síntese química , Pirimidinas/farmacologia , Tiazóis/síntese química , Tiazóis/farmacologia , Antineoplásicos/química , Linhagem Celular Tumoral , Proliferação de Células/efeitos dos fármacos , Dasatinibe , Relação Dose-Resposta a Droga , Ensaios de Seleção de Medicamentos Antitumorais , Humanos , Estrutura Molecular , Pirimidinas/química , Estereoisomerismo , Relação Estrutura-Atividade , Tiazóis/química
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