41 research outputs found

    Multiple-Responsive Hierarchical Self-Assemblies of a Smart Supramolecular Complex: Regulation of Noncovalent Interactions

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    We herein report a smart amphiphilic supramolecular complex ([MimA–EDA–MimA]@[DBS]<sub>2</sub>) with stimuli-responsive self-assembly, constructed by 3-(3-formyl-4-hydroxybenzyl)-1-methylimidazolium chloride (MimACl), sodium dodecyl benzene sulfonate (SDBS), and ethylenediamine (EDA). The self-assembly of [MimA–EDA–MimA]@[DBS]<sub>2</sub> shows triple-sensitivities in response to pH, concentration, and salt. At a low pH, only micelles are formed, which can transform into vesicles spontaneously when the pH increases to 11.8. Vesicles can gradually fuse into vesicle clusters and elongated assemblies with increasing concentration of [MimA–EDA–MimA]@[DBS]<sub>2</sub>. Chainlike aggregates, ringlike aggregates, or giant vesicles can be formed by adding inorganic salts (i.e., NaCl and NaNO<sub>3</sub>), which could be derived from the membrane fusion of vesicles. The noncovalent interactions, including π–π stacking, hydrogen bonding, and electrostatic interactions, were found to be responsible for the topology evolution of assemblies. Thus, it provides an opportunity to construct smart materials through the regulation of the role of noncovalent interactions in self-assembly

    DNA Assembled Gold Nanoparticles Polymeric Network Blocks Modular Highly Sensitive Electrochemical Biosensors for Protein Kinase Activity Analysis and Inhibition

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    A highly sensitive electrochemical biosensor was built for the detection of kinase activity based on the DNA induced gold nanoparticles (AuNPs) polymeric network block signal amplification. In this strategy, the DNA<sub>1</sub> conjugated AuNPs were integrated with the phosphorylated peptide by Zr<sup>4+</sup> and assembled into DNA-AuNPs polymeric network block by the hybridization of cDNA with each side sequences of DNA<sub>1</sub> and joint DNA<sub>2</sub>. The kinase activity was determined by the amperometric responses of [Ru­(NH<sub>3</sub>)<sub>6</sub>]<sup>3+</sup> absorbed on the network block by electrostatic interaction. Due to its excellent electroactivity and high accommodation of the DNA-AuNPs polymeric network block for [Ru­(NH<sub>3</sub>)<sub>6</sub>]<sup>3+</sup>, the current signal was significantly amplified, affording a highly sensitive electrochemical analysis of kinase activity. The as-proposed biosensor presents a low detection limit of 0.03 U mL<sup>–1</sup> for protein kinase A (PKA) activity, wide linear range (from 0.03 to 40 U mL<sup>–1</sup>), and excellent stability even in cell lysates and serum samples. This biosensor can also be applied for quantitative kinase inhibitor screening. Finally, the PKA activities from BE4S-2B, A549, and MCF-7 cell lysates were further analyzed, which provided a valuable strategy in developing a high-throughput assay of in vitro kinase activity and inhibitor screening for clinic diagnostics and therapeutics

    Integrating a Silicon Solar Cell with a Triboelectric Nanogenerator <i>via</i> a Mutual Electrode for Harvesting Energy from Sunlight and Raindrops

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    Solar cells, as promising devices for converting light into electricity, have a dramatically reduced performance on rainy days. Here, an energy harvesting structure that integrates a solar cell and a triboelectric nanogenerator (TENG) device is built to realize power generation from both sunlight and raindrops. A heterojunction silicon (Si) solar cell is integrated with a TENG by a mutual electrode of a poly­(3,4-ethylenedioxythiophene):poly­(styrenesulfonate) (PEDOT:PSS) film. Regarding the solar cell, imprinted PEDOT:PSS is used to reduce light reflection, which leads to an enhanced short-circuit current density. A single-electrode-mode water-drop TENG on the solar cell is built by combining imprinted polydimethylsiloxane (PDMS) as a triboelectric material combined with a PEDOT:PSS layer as an electrode. The increasing contact area between the imprinted PDMS and water drops greatly improves the output of the TENG with a peak short-circuit current of ∼33.0 nA and a peak open-circuit voltage of ∼2.14 V, respectively. The hybrid energy harvesting system integrated electrode configuration can combine the advantages of high current level of a solar cell and high voltage of a TENG device, promising an efficient approach to collect energy from the environment in different weather conditions

    Lithium-Containing Zwitterionic Poly(Ionic Liquid)s as Polymer Electrolytes for Lithium-Ion Batteries

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    Polymer electrolytes are considered as the good candidates for the new-generation-safe lithium-ion battery. Herein, a free-standing and flexible polymer electrolyte film based on a lithium-containing zwitterionic poly­(ionic liquid) (PIL) was constructed with and without propylene carbonate (PC) by in-situ photopolymerization. In this system, the lithium-containing IL synthesized by equimolecular neutralization of imidazolium-type zwitterion 3-(1-vinyl-3-imidazolio)­propanesulfonate (VIPS) and lithium bis­(trifluoromethylsulfonyl)­imide (LiTFSI) can both serve as the polymeric matrix of the polymer electrolytes to maintain sufficient mechanical strength and form Li<sup>+</sup>-rich channels for lithium-ion transportation. The ion–dipole interaction between the lithium ion and the polar solvent PC can further improve the lithium-ion conduction, resulting in a comparable ionic conductivity of ∼10<sup>–3</sup> S/cm at 30 °C. Charge–discharge cycling performance of Li/LiFePO<sub>4</sub> half-cell equipped with the PIL-based polymer electrolyte indicates the possibility of practical application. Simultaneously, the lithium-containing zwitterionic PIL fabricated by this facile method provides a promising model system for understanding the molecular interactions in promoting the lithium-ion conduction

    Rhodomollacetals A–C, PTP1B Inhibitory Diterpenoids with a 2,3:5,6-Di-<i>seco</i>-grayanane Skeleton from the Leaves of <i>Rhododendron molle</i>

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    Three novel diterpenoids with an unprecedented 2,3:5,6-di-<i>seco</i>-grayanane carbon skeleton, rhodomollacetals A–C (<b>1</b>–<b>3</b>), are isolated from the leaves of <i>Rhododendron molle</i>. Their structures are elucidated by comprehensive spectroscopic techniques and single-crystal X-ray diffraction. Rhodomollacetal A (<b>1</b>) possesses a novel <i>cis/cis/cis/cis</i>-fused 6/6/6/6/5 pentacyclic ring system, featuring an unprecedented 11,13,18-trioxa-pentacyclo [8.7.1.1<sup>5,8</sup>.0<sup>2,8</sup>.0<sup>12,17</sup>]­nonadecane scaffold. Compounds <b>2</b> and <b>3</b> have a rare 4-oxatricyclo­[7.2.1.0<sup>1,6</sup>]­dodecane moiety and a 2,3-dihydro-4<i>H</i>-pyran-4-one unit. Compounds <b>1</b>–<b>3</b> showed moderate PTP1B inhibitory activities, and their molecular dockings were investigated

    Two new 1-D and 3-D Wells–Dawson structures assisted by alkali metals

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    <div><p>Two new Wells–Dawson based compounds containing alkali metals, [Ag(H<sub>2</sub>biim)<sub>2</sub>]<sub>2</sub>·[Ag<sub>5</sub>(H<sub>2</sub>biim)<sub>10</sub>Na<sub>2</sub>(H<sub>2</sub>O)<sub>2</sub>(H<sub>3/2</sub>P<sub>2</sub>W<sub>18</sub>O<sub>62</sub>)<sub>2</sub>]·12H<sub>2</sub>O (<b>1</b>) and [Cd(H<sub>2</sub>biim)<sub>2</sub> K(P<sub>2</sub>W<sub>18</sub>O<sub>62</sub>)<sub>1/2</sub>] (<b>2</b>) (H<sub>2</sub>biim = 2,2′-biimidazole), have been synthesized under hydrothermal conditions. In <b>1</b>, two-supporting Wells–Dawson anions are linked by a [Ag(H<sub>2</sub>biim)<sub>2</sub>]<sup>+</sup> subunit to form a dimer. The adjacent dimers are further connected by Na<sup>+</sup> through (POM)O-Na-O(POM) bonds to build a 1-D chain. In <b>2</b>, adjacent anions are linked by two [Cd<sub>2</sub>(H<sub>2</sub>biim)<sub>2</sub>]<sup>4+</sup> subunits and a 1-D chain is formed. Furthermore, the anion in the chain is fused by six K<sup>+</sup> ions and a 3-D framework is obtained. The alkali metals exhibit crucial influence on the conversion of dimensionality assisting anions and Ag-H<sub>2</sub>biim subunits to construct 1-D and 3-D frameworks. The electrochemical and photocatalytic properties of <b>1</b> and <b>2</b> have been investigated.</p></div

    Near-Infrared Light-Driven Photoelectrochemical Aptasensor Based on the Upconversion Nanoparticles and TiO<sub>2</sub>/CdTe Heterostructure for Detection of Cancer Cells

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    A near-infrared-driven photoelectrochemical aptasensor was developed as a new method for the detection of the breast cancer cell MCF-7. The upconversion nanoparticles and TiO<sub>2</sub>/CdTe heterostructure were combined to prepare the film electrode, and the high-affinity aptamer AS1411 was conjugated to the electrode to recognize MCF-7 cells. In this fabrication, the upconversion nanoparticles transferred the near-infrared light to visible light, which could excite the semiconductor to enhance the current response. As a result, the aptasensor revealed good sensitivity and specificity with MCF-7 cell concentrations ranging from 1 × 10<sup>3</sup> to 1 × 10<sup>5</sup> cells/mL. The results presented a favorable determination of MCF-7 cells, which was achieved with the help of the upconversion nanoparticles and the photoelectrochemical interface

    Waterproof, Breathable, and UV-Protective Nanofiber-Based Triboelectric Nanogenerator for Self-Powered Sensors

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    Nanofiber-based triboelectric nanogenerators (TENGs) have garnered increasing attention as the multifunctional power source in wearable electronics. However, most traditional wearable device-based TENGs are unable to simultaneously achieve excellent outputs and multifunctional properties. Here, we design a waterproof, breathable, UV-protective TENG based on a poly(vinylidene fluoride) (PVDF)/poly(dimethylsiloxane) (PDMS)/TiO2 nanofiber film for effective harvesting mechanical energy by a simple and low-cost combined electrospinning/electrospray method. The introduction of PVDF can overcome the synthesis puzzle of PDMS nanofibers during the electrospinning process. With numerous three-dimensional micro-to-nano hierarchical pores of a nanofiber network, the constructed TENG can furnish large specific surface area and good breathability. The addition of TiO2 nanoparticles (NPs) increases the dielectric constant and surface roughness of the PVDF/PDMS/TiO2 nanofiber film as well as the corresponding output performance of the nanofiber-based TENG. The as-presented TENG has a maximum peak power density of 0.72 W/m2 and excellent breathability (18.6 mm/s). Due to the UV radiation absorbed by the TiO2 NPs, the UVA transmittance (TUVA) of the TENG with 4% TiO2 NPs is decreased to only 8.2%. The constructed TENG can be integrated to monitor human physiological signals in a self-powered manner. The nanofiber-based TENG provides a version to render these suitable for the daily-used wearable or portable electronics shortly
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