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1.
Anal Chem ; 2024 May 10.
Artículo en Inglés | MEDLINE | ID: mdl-38728651

RESUMEN

In the realm of nanopore sensor technology, an enduring challenge lies in achieving the discerning detection of small biomolecules with a sufficiently high signal-to-noise ratio. This study introduces a method for reliably quantifying the concentration of target small molecules, utilizing tetrahedral DNA nanostructures as surrogates for the captured molecules through a magnetic-bead-based competition substitution mechanism. Magnetic Fe3O4-DNA tetrahedron nanoparticles (MNPs) are incorporated into a nanopore electrochemical system for small-molecule sensing. In the presence of the target, the DNA tetrahedron, featuring an aptamer tail acting as a molecular carrier, detaches from the MNPs due to aptamer deformation. Following removal of the MNPs, the DNA tetrahedron bound to the target traversed the nanopore by applying a positive potential. This approach exhibits various advantages, including heightened sensitivity, selectivity, an improved signal-to-noise ratio (SNR), and robust anti-interference capabilities. Our findings demonstrate that this innovative methodology has the potential to significantly enhance the sensing of various small-molecule targets by nanopores, thereby advancing the sensitivity and dynamic range. This progress holds promise for the development of precise clinical diagnostic tools.

2.
Heliyon ; 10(10): e30909, 2024 May 30.
Artículo en Inglés | MEDLINE | ID: mdl-38778961

RESUMEN

Background: Observational studies have found a potential link between the use of thiazolidinediones (TZDs) and a lower risk of Alzheimer's disease (AD) development. Platelets were the great source of amyloid-ß (Aß) and involved in the development of AD. This study aimed to assess the correlation between antidiabetic agents and platelet characteristics, hoping to provide a potential mechanism of TZDs neuroprotection in AD. Method: Drug-targeted Mendelian randomization (MR) was performed to systematically illustrate the long-term effects of antidiabetic agents on platelet characteristics. Four antidiabetic agent targets were considered. Positive control analysis for type 2 diabetes (T2D) was conducted to validate the selection of instrumental variables (IVs). Colocalization analysis was used to further strengthen the robustness of the results. Result: Positive control analysis showed an association of four antidiabetic agents with lower risk of T2D, which was consistent with their mechanisms of action and previous evidence from clinical trials. Genetically proxied TZDs were associated with lower platelet count (ß[IRNT] = -0.410 [95 % CI -0.533 to -0.288], P = 5.32E-11) and a lower plateletcrit (ß[IRNT] = -0.344 [95 % CI -0.481 to -0.206], P = 1.04E-6). Colocalization suggested the posterior probability of hypothesis 4 (PPH4) > 0.8, which further strengthened the MR results. Conclusion: Genetically proxied TZDs were causally associated with lower platelet characteristics, particularly platelet count and plateletcrit, providing insight into the involvement of platelet-related pathways in the neuroprotection of TZDs against AD. Future studies are warranted to reveal the underlying molecular mechanism of TZDs' neuroprotective effects through platelet pathways.

3.
Front Microbiol ; 15: 1342653, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-38585702

RESUMEN

Background: Inflammation serves as a key pathologic mediator in the progression of infections and various diseases, involving significant alterations in the gut microbiome and metabolism. This study aims to probe into the potential causal relationships between gut microbial taxa and human blood metabolites with various serum inflammatory markers (CRP, SAA1, IL-6, TNF-α, WBC, and GlycA) and the risks of seven common infections (gastrointestinal infections, dysentery, pneumonia, bacterial pneumonia, bronchopneumonia and lung abscess, pneumococcal pneumonia, and urinary tract infections). Methods: Two-sample Mendelian randomization (MR) analysis was performed using inverse variance weighted (IVW), maximum likelihood, MR-Egger, weighted median, and MR-PRESSO. Results: After adding other MR models and sensitivity analyses, genus Roseburia was simultaneously associated adversely with CRP (Beta IVW = -0.040) and SAA1 (Beta IVW = -0.280), and family Bifidobacteriaceae was negatively associated with both CRP (Beta IVW = -0.034) and pneumonia risk (Beta IVW = -0.391). After correction by FDR, only glutaroyl carnitine remained significantly associated with elevated CRP levels (Beta IVW = 0.112). Additionally, threonine (Beta IVW = 0.200) and 1-heptadecanoylglycerophosphocholine (Beta IVW = -0.246) were found to be significantly associated with WBC levels. Three metabolites showed similar causal effects on different inflammatory markers or infectious phenotypes, stearidonate (18:4n3) was negatively related to SAA1 and urinary tract infections, and 5-oxoproline contributed to elevated IL-6 and SAA1 levels. In addition, 7-methylguanine showed a positive correlation with dysentery and bacterial pneumonia. Conclusion: This study provides novel evidence confirming the causal effects of the gut microbiome and the plasma metabolite profile on inflammation and the risk of infection. These potential molecular alterations may aid in the development of new targets for the intervention and management of disorders associated with inflammation and infections.

4.
Small ; : e2400796, 2024 Apr 12.
Artículo en Inglés | MEDLINE | ID: mdl-38607275

RESUMEN

Solar-driven interfacial evaporation (SDIE) is a highly promising approach to achieve sustainable desalination and tackle the global freshwater crisis. Despite advancements in this field, achieving balanced thermal localization and salt resistance remains a challenge. Herein, the study presents a 3D hierarchical porous ceramic platform for SDIE applications. The utilized alumina foam ceramics (AFCs) exhibit remarkable corrosion resistance and chemical stability, ensuring a prolonged operational lifespan in seawater or brines. The millimeter-scale air-filled pores in AFCs prevent thermal losses through conduction with bulk water, resulting in heat-localized interfaces. The hydrophilic nature of macroporous AFC skeletons facilitates rapid water replenishment on the evaporating surface for effective salt-resistant desalination. Benefiting from its self-radiation adsorption and side-assisted evaporation capabilities, the AFC-based evaporators exhibit high indoor evaporation rates of 2.99 and 3.54 kg m-2 h-1 under one-sided and three-sided illumination under 1.0 sun, respectively. The AFC-based evaporator maintains a high evaporation rate of ≈2.77 kg m-2 h-1 throughout the 21-day long-term test. Furthermore, it achieves a daily water productivity of ≈10.44 kg m-2 in outdoor operations. This work demonstrates the potential of 3D hierarchical porous ceramics in addressing the trade-off between heat localization and salt resistance, and contributes to the development of durable solar steam generators.

5.
Org Lett ; 26(15): 2918-2922, 2024 Apr 19.
Artículo en Inglés | MEDLINE | ID: mdl-38560790

RESUMEN

The asymmetric total syntheses of ent-stachybotrin C and its congener have been accomplished through a convergent approach in the longest linear sequence of 12 steps from commercially available materials, respectively. Noteworthy transformation of the synthesis involved a cascade Knoevenagel condensation/Hantzsch ester reduction/epoxide ring-opening/transetherification to construct the core pyran ring with two adjacent stereocenters.

6.
Polymers (Basel) ; 16(8)2024 Apr 21.
Artículo en Inglés | MEDLINE | ID: mdl-38675086

RESUMEN

Marine anti-fouling coatings represent an efficient approach to prevent and control the marine biofouling. However, a significant amount of antifouling agent is added to improve the static antifouling performance of the coatings, which leads to an issue whereby static antifouling performance conflicts with eco-friendly traits. Herein, this work reports an in situ reduction synthesis of silver nanoparticles (AgNPs) within polymers to produce composite coatings, aiming to solve the aforementioned issue. Firstly, urushiol-based benzoxazine monomers were synthesized by the Mannich reaction, using an eco-friendly natural product urushiol and n-octylamine and paraformaldehyde as the reactants. Additionally, AgNPs were obtained through the employment of free radicals formed by phenolic hydroxyl groups in the urushiol-based benzoxazine monomers, achieved by the in situ reduction of silver nitrate in benzoxazine. Then, the urushiol-based benzoxazine/AgNPs composite coatings were prepared by the thermosetting method. AgNPs exhibit broad-spectrum and highly efficient antimicrobial properties, with a low risk to human health and a minimal environmental impact. The composite coating containing a small amount of AgNPs (≤1 wt%) exhibits effective inhibition against various types of bacteria and marine microalgae in static immersion, thereby displaying outstanding antifouling properties. This organic polymer and inorganic nanoparticle composite marine antifouling coating, with its simple preparation method and eco-friendliness, presents an effective solution to the conflict between static antifouling effectiveness and environmental sustainability in marine antifouling coatings.

7.
Waste Manag ; 174: 88-95, 2024 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-38035661

RESUMEN

With the extensive use of lithium-ion batteries (LIBs), neglecting to recycle graphite anodes from LIBs leads to environmental pollution and the waste of graphite resources. Thus, developing an efficient and environment-protecting approach to reusing spent graphite anodes is necessary. Here, high value-added graphene sheets (GS), carbon nanohorns (CNHs), fluorine-doped CNHs (F-CNHs), and amorphous carbon nanoballs (ACNs) were prepared from spent graphite anodes of LIBs via DC arc plasma. In order to control the conversion of spent graphite anodes into various carbon nanomaterials, the growth mechanism of carbon nanomaterials is investigated by quenching rate. Benefiting from the extremely high quenching rates (>1.8 × 106 K/s) produced by DC arc plasma, the particle size of the prepared ACNs and CNHs is small and evenly distributed. The CNHs show a "dahlia-like" structure, and the number of graphene layers is only 3-8. Furthermore, the structural transformation mechanism of carbon nanomaterials is researched by deposition temperature. The ACNs, few-layer GS, and CNHs produced by the high quenching rates are unstable and prone to structural transformation. When these carbon nanomaterials are deposited on the cathode surface and cathode holder, the ACNs, "dahlia-like" CNHs, and GS undergo processes of fusing and overlaying at high temperatures, respectively, resulting in the agglomeration and increased particle size of ACNs and "seed-like" CNHs. Meanwhile, the GS is bent and converted into carbon nanocages (CBCs). Overall, the carbon nanomaterials prepared using spent anodes from LIBs by arc plasma are a facile, environment-friendly, and economical strategy to achieve high value-added utilization of the graphite.


Asunto(s)
Grafito , Nanoestructuras , Grafito/química , Carbono/química , Litio/química , Iones , Nanoestructuras/química , Electrodos
8.
Materials (Basel) ; 16(23)2023 Dec 01.
Artículo en Inglés | MEDLINE | ID: mdl-38068213

RESUMEN

Nanostructured transition metal nitrides (TMNs) have been considered as a promising substitute for precious metal catalysts toward ORR due to their multi-electron orbitals, metallic properties, and low cost. To design TMN catalysts with high catalytic activity toward ORR, the intrinsic features of the influencing factor on the catalytic activity toward ORR of nanostructured TMNs need to be investigated. In this paper, titanium nitride (TiN), zirconium nitride (ZrN), and hafnium nitride (HfN) nanoparticles (NPs) are highly efficient and synthesized in one step by the direct current arc plasma. TiN, ZrN, and HfN NPs with an oxidation layer are applied as the catalysts of hybrid sodium-air batteries (HSABs). The effect of the composition and structural attributes of TMNs on ORR catalysis is defined as follows: (i) composition effect. With the increase in the oxygen content, the catalytic ORR capability of TMNs decreases progressively due to the reduction in oxygen adsorption capacity; (ii) structure effect. The redistribution of the density of states (DOS) of ZrN indicates higher ORR activity than TiN and HfN. HSABs with ZrN exhibit an excellent cyclic stability up to 137 cycles (about 140 h), an outstanding rate performance, and a specific capacity of 2817 mAh·g-1 at 1.0 mA·cm-2.

9.
Nat Commun ; 14(1): 6891, 2023 Oct 28.
Artículo en Inglés | MEDLINE | ID: mdl-37898686

RESUMEN

Developing efficient artificial photocatalysts for the biomimetic photocatalytic production of molecular materials, including medicines and clean energy carriers, remains a fundamentally and technologically essential challenge. Hydrogen peroxide is widely used in chemical synthesis, medical disinfection, and clean energy. However, the current industrial production, predominantly by anthraquinone oxidation, suffers from hefty energy penalties and toxic byproducts. Herein, we report the efficient photocatalytic production of hydrogen peroxide by protonation-induced dispersible porous polymers with good charge-carrier transport properties. Significant photocatalytic hydrogen peroxide generation occurs under ambient conditions at an unprecedented rate of 23.7 mmol g-1 h-1 and an apparent quantum efficiency of 11.3% at 450 nm. Combined simulations and spectroscopies indicate that sub-picosecond ultrafast electron "localization" from both free carriers and exciton states at the catalytic reaction centers underlie the remarkable photocatalytic performance of the dispersible porous polymers.

10.
Molecules ; 28(18)2023 Sep 20.
Artículo en Inglés | MEDLINE | ID: mdl-37764484

RESUMEN

Developing robust and cost-effective electrocatalysts to boost hydrogen evolution reactions (HERs) and oxygen evolution reactions (OERs) is crucially important to electrocatalytic water splitting. Herein, bifunctional electrocatalysts, by coupling Co nanoparticles and N-doped carbon nanotubes/graphitic nanosheets (Co@NCNTs/NG), were successfully synthesized via facile high-temperature pyrolysis and evaluated for water splitting. The morphology and particle size of products were influenced by the precursor type of the cobalt source (cobalt oxide or cobalt nitrate). The pyrolysis product prepared using cobalt oxide as a cobalt source (Co@NCNTs/NG-1) exhibited the smaller particle size and higher specific surface area than that of the pyrolysis products prepared using cobalt nitrate as a cobalt source (Co@NCNTs/NG-2). Notably, Co@NCNTs/NG-1 displayed much lower potential -0.222 V vs. RHE for HER and 1.547 V vs. RHE for OER at the benchmark current density of 10 mA cm-2 than that of Co@NCNTs/NG-2, which indicates the higher bifunctional catalytic activities of Co@NCNTs/NG-1. The water-splitting device using Co@NCNTs/NG-1 as both an anode and cathode demonstrated a potential of 1.92 V to attain 10 mA cm-2 with outstanding stability for 100 h. This work provides a facile pyrolysis strategy to explore highly efficient and stable bifunctional electrocatalysts for water splitting.

11.
Environ Res ; 238(Pt 1): 117071, 2023 12 01.
Artículo en Inglés | MEDLINE | ID: mdl-37669736

RESUMEN

As the accumulation of waste tires continues to rise year by year, effectively managing and recycling these discarded materials has become an urgent global challenge. Among various potential solutions, pyrolysis stands out due to its superior environmental compatibility and remarkable efficiency in transforming waste tires into valuable products. Thus, it is considered the most potential method for disposing these tires. In this work, waste tire powder is pyrolyzed at 560 °C to yield pyrolysis carbon black, and meanwhile, the purification effects of base-acid solutions on pyrolysis carbon black are discussed. High-purity few-layer graphene flakes and carbon nanohorns are synthesized by a direct current arc plasma with H2 and N2 as buffer gases and high-purity pyrolysis carbon black as raw material. Under an H2 atmosphere, hydrogen effectively terminates the suspended carbon bonds, preventing the formation of closed structures and facilitating the expansion of graphene sheets. During the preparation of carbon nanohorns, the nitrogen atoms rapidly bond with carbon atoms, forming essential C-N bonds. This nitrogen doping promotes the formation of carbon-based five-membered and seven-membered rings and makes the graphite lamellar change in the direction of towards negative curvature. Consequently, such change facilitates the formation of conical structures, ultimately yielding the coveted carbon nanohorns. This work not only provides an economical raw material for efficient large-scale synthesis of few-layer graphene and carbon nanohorns but also broadens the intrinsic worth of pyrolysis carbon black, which is beneficial to improving the recycling value of waste tires.


Asunto(s)
Grafito , Carbono , Hollín , Temperatura , Nitrógeno
12.
Nanomaterials (Basel) ; 13(4)2023 Feb 13.
Artículo en Inglés | MEDLINE | ID: mdl-36839083

RESUMEN

Carbon-encapsulated transition metal catalysts have caught the interest of researchers in the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) due to their distinctive architectures and highly tunable electronic structures. In this work, we synthesized N-doped carbon encapsulated with CoNi nanoalloy particles (CoNi@NC) as the electrocatalysts. The metal-organic skeleton ZIF-67 nanocubes were first synthesized, and then Ni2+ ions were inserted to generate CoNi-ZIF precursors by a simple ion-exchange route, which was followed by pyrolysis and with urea for the introduction of nitrogen (N) at a low temperature to synthesize CoNi@NC composites. The results reveal that ZIF-67 pyrolysis can dope more N atoms in the carbon skeleton and that the pyrolysis temperature influences the ORR and OER performances. The sample prepared by CoNi@NC pyrolysis at 650 °C has a high N content (9.70%) and a large specific surface area (167 m2 g-1), with a positive ORR onset potential (Eonset) of 0.89 V vs. RHE and half-wave potential (E1/2) of 0.81 V vs. RHE in 0.1 M KOH, and the overpotential of the OER measured in 1 M KOH was only 286 mV at 10 mA cm-2. The highly efficient bifunctional ORR/OER electrocatalysts synthesized by this method can offer some insights into the design and synthesis of complex metal-organic frameworks (MOFs) hybrid structures and their derivatives as functional materials in energy storage.

13.
Chem Asian J ; 17(20): e202200645, 2022 Oct 17.
Artículo en Inglés | MEDLINE | ID: mdl-35982529

RESUMEN

Direct Z-scheme Cu7 S4 /CdS Janus photocatalysts are successfully prepared by cation exchange method. Extensive studies containing single-nanoparticle impact electrochemistry are performed and reveal that optimizing the Cu7 S4 /CdS ratio can decrease the accumulation of holes on valence band of CdS for inhibiting photo-corrosion and promote the accumulation of electrons on the conduction band of Cu7 S4 for boosting the electron reducibility. With the optimized heterostructures, hydrogen evolution is remarkable promoted up to 21.62 mmol/g/h and quantum efficiency is up to 14.37% using polylactic acid plastic waste as feedstock.


Asunto(s)
Procesos Fotoquímicos , Sulfuros , Sulfuros/química , Catálisis , Hidrógeno/química , Plásticos
14.
Nat Commun ; 13(1): 1402, 2022 03 17.
Artículo en Inglés | MEDLINE | ID: mdl-35301326

RESUMEN

The fascinating phenomenon that plasmon excitation can convert isotropic silver nanospheres to anisotropic nanoprisms has already been developed into a general synthetic technique since the discovery in 2001. However, the mechanism governing the morphology conversion is described with different reaction processes. So far, the mechanism based on redox reactions dominated anisotropic growth by plasmon-produced hot carriers is widely accepted and developed. Here, we successfully achieved plasmon-driven high yield conversion of gold nanospheres into nanoplates with iodine as the inducer. To investigate the mechanism, nanopore sensing technology is established to statistically study the intermediate species at the single-nanoparticle level. Surprisingly, the morphology conversion is proved as a hot hole-controlled coalescence-dominated growth process. This work conclusively elucidates that a controllable plasmon-driven nanoparticle-coalescence mechanism could enable the production of well-defined anisotropic metal nanostructures and suggests that the nanopore sensing could be of general use for studying the growth process of nanomaterials.


Asunto(s)
Nanopartículas del Metal , Nanoporos , Oro/química , Nanopartículas del Metal/química , Plata/química , Resonancia por Plasmón de Superficie/métodos
15.
ACS Appl Mater Interfaces ; 13(8): 9771-9780, 2021 Mar 03.
Artículo en Inglés | MEDLINE | ID: mdl-33615775

RESUMEN

In perovskite solar cells, the halide vacancy defects on the perovskite film surface/interface will instigate charge recombination, leading to a decrease in cell performance. In this study, cadmium sulfide (CdS) has been introduced into the precursor solution to reduce the halide vacancy defects and improve the cell performance. The highest efficiency of the device reaches 21.62%. Density functional theory calculation reveals that the incorporated Cd2+ ions can partially replace Pb2+ ions, thus forming a strong Cd-I bond and effectively reducing iodide vacancy defects (VI); at the same time, the loss of the charge recombination is significantly reduced because VI is filled by S2- ions. Besides, the substitution of Cd2+ for Pb2+ could increase the generation of PbI2, which can further passivate the grain boundary. Therefore, the stability of the cells, together with the efficiency of the power conversion efficiencies (PCEs), is also improved, maintaining 87.5% of its initial PCEs after being irradiated over 410 h. This work provides a very effective strategy to passivate the surface/interface defects of perovskite films for more efficient and stable optoelectronic devices.

16.
Chemistry ; 27(3): 939-943, 2021 Jan 13.
Artículo en Inglés | MEDLINE | ID: mdl-32935405

RESUMEN

Construction of local donor-acceptor architecture is one of the valid means for facilitating the intramolecular charge transfer in organic semiconductors. To further accelerate the interface charge transfer, a ternary acceptor-donor-acceptor (A1 -D-A2 ) molecular junction is established via gradient nitrogen substituting into the polymer skeleton. Accordingly, the exciton splitting and interface charge transfer could be promptly liberated because of the strong attracting ability of the two different electron acceptors. Both DFT calculations and photoluminescence spectra elucidate the swift charge transfer at the donor-acceptor interface. Consequently, the optimum polymer, N3 -CP, undergoes a remarkable photocatalytic property in terms of hydrogen production with AQY405 nm =26.6 % by the rational design of asymmetric molecular junctions on organic semiconductors.

17.
Molecules ; 25(23)2020 Dec 04.
Artículo en Inglés | MEDLINE | ID: mdl-33291521

RESUMEN

In our previous study, temporin-GHaR (GHaR) showed potent antimicrobial activity with strong hemolytic toxicity. To overcome its weakness, we designed GHaR6R, GHaR7R, GHaR8R, GHaR9R, and GHaR9W by changing the number of positive charges and the hydrophobic surface of GHaR. With the exception of GHaR7R, the hemolytic toxicity of the derived peptides had been reduced, and the antimicrobial activities remained close to the parent peptide (except for GHaR9R). GHaR6R, GHaR7R, GHaR8R, and GHaR9W exhibited a great bactericidal effect on Streptococcus mutans (S. mutans), which is one of the main pathogens causing dental caries. According to the membrane permeation and scanning electron microscope (SEM) analysis, these derived peptides targeted to the cell membranes of planktonic bacteria, contributing to the disruption of the membrane integrity and leakage of the intracellular contents. Moreover, they inhibited the formation of biofilms and eradicated the mature biofilms of S. mutans. Compared with GHaR7R, the derived peptides showed less cytotoxicity to human oral epithelial cells (HOECs). The derived peptides are expected to be the molecular templates for designing antibacterial agents to prevent dental caries.


Asunto(s)
Antiinfecciosos/farmacología , Péptidos Catiónicos Antimicrobianos/farmacología , Biopelículas/efectos de los fármacos , Hemólisis/efectos de los fármacos , Péptidos/farmacología , Streptococcus mutans/efectos de los fármacos , Membrana Celular/microbiología , Caries Dental/microbiología , Células Epiteliales/microbiología , Eritrocitos/microbiología , Humanos , Pruebas de Sensibilidad Microbiana/métodos
18.
Talanta ; 219: 121213, 2020 Nov 01.
Artículo en Inglés | MEDLINE | ID: mdl-32887115

RESUMEN

The abuse of adamantanamine (ADA) and its derivatives as veterinary drugs in the poultry industry could cause severe health problems for humans. It is of great need to develop a rapid, cheap and ultrasensitive method for ADA detection. In this study, a sensitive conical nanochannel sensor was established for the rapid quantitative detection of ADA with the distinctive design of the host-guest competition. The sensor was constructed by functionalizing the nanochannel surface with p-toluidine and was then assembled with Cucurbit [7]uril (CB [7]). When ADA is added, it could occupy the cavity of CB [7] due to the host-guest competition and makes CB [7] to release from the CB [7]-p-toluidine complex, resulting in a distinct change of hydrophobicity of the nanochannel, which could be determined by the ionic current. Under the optimal conditions, the strategy permitted sensitive detection of ADA in a linear range of 10-1000 nM. The nanochannel based ADA sensing platform showed both high sensitivity and excellent reproducibility and the limit of detection was 4.54 nM. For the first time, the rapid and sensitive recognition of an illegal medicine was realized based on the host-guest competition method with the nanochannel system and the principle and feasibility of this method were described at length. This strategy provides a simple, reliable, and effective way to apply host-guest system in the development of nanochannel sensor for small-molecule drug detection.

19.
ACS Appl Mater Interfaces ; 12(29): 32514-32525, 2020 Jul 22.
Artículo en Inglés | MEDLINE | ID: mdl-32578976

RESUMEN

Although nanostructured materials have recently enabled a dramatic improvement of the current energy-storage units in portable electronics with enhanced functionality, it is still challenging to provide a cost-efficient solution to attain the ultrahigh energy and power densities of supercapacitors (SCs) since nearly arbitrary electrodes are limited to the thinner porous structure with de facto rather low mass loading (∼1 mg cm-2) because of the huge limitations of pronounced impaired ion transport in subnanometer pores in thicker compact electrodes. In this contribution, we report the fabrication of a macro/mesoporous hybrid hierarchical nanocomposite SiC/holey-graphene/holey-MnO2 (SiC/HG/h-MnO2) with tailored porosity by knitting together the quasi-aligned single-crystalline doped 3C-SiC nanowire array and in situ surface-reduced holey graphene framework into a three-dimensional quasi-ordered structure, which enables the mass growth of ultrathin h-MnO2 nanosheets at approximately practical levels of mass loading. The produced synergistically favorable interconnected porous architecture allows for the highly efficient electron transfer and rapid ion transport up to interior surfaces of the network. Remarkably, the all-solid-state flexible asymmetric supercapacitors (ASCs) made with SiC/HG/h-MnO2 and SiC/graphitic carbon (GC) nanoarrays are mechanically robust and show a high areal capacity (0.32 mWh cm-2) and a high rate capability (280 mW cm-2) at ultrahigh mass loading (6.5 mg cm-2), much higher than most of previous superior SCs in aqueous or gelled electrolytes and thus offer an entirely new prototype of textile-based ASCs, which represents a critical step toward practical applications for various portable electronics.

20.
J Org Chem ; 85(8): 5724-5732, 2020 04 17.
Artículo en Inglés | MEDLINE | ID: mdl-32212620

RESUMEN

The nominal enantiomer of chlorabietol B was regio- and stereoselectively synthesized from (-)-abietic acid in 13 steps. Key features of the synthesis involved an oxidative [3+2] cycloaddition to install the dihydrobenzofuran moiety and an Aldol reaction, followed by elimination and reduction steps to introduce the long chain with three cis double bonds. However, obvious differences in the NMR spectra of the synthetic and natural samples suggested that the proposed structure of chlorabietol B should be revised carefully.

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