Latest ArticlesAll solid-state lithium metal batteries (ASSLMBs) based on polymer solid electrolyte and lithium metal anode have attracted much attention due to their high energy density and intrinsic safety. However, the low ionic conductivity at room temperature and poor mechanical properties of the solid polymer electrolyte result in increased polarization and poor cycling stability of the Li metal batteries. In order to improve the ionic conductivity at room temperature while maintaining mechanical strength, we combine the conductivity of short chain polyethylene oxide (PEO) and strength of styrene-maleic anhydride copolymer (SMA) to obtain a grafted block copolymer with nanophase separation structure, which has room temperature ionic conductivity up to 1.14 × 10−4 S/cm and tensile strength up to 1.4 MPa. Li||Li symmetric cell can work stably for more than 1500 h under the condition of 0.1 mA/cm2. Li||LiFePO4 full cells can deliver a high capacity of 151.4 mAh/g at 25 ℃ and 0.2 C/0.2 C charge/discharge conditions, showing 85.6% capacity retention after 400 cycles. Importantly, the all solid state Li||LiFePO4 pouch cell shows excellent safety performance under different abuse conditions. These results demonstrate that the nanophase separated, grafted alternate copolymer electrolyte has huge potential for application in Li metal batteries.
Photothermal therapy (PTT) and photodynamic therapy (PDT) have received tremendous attention owing to their great potential for tumor treatment. However, two main issues hamper the antitumor performance of PDT: overexpression of glutathione (GSH) in tumors, which consumes PDT-induced reactive oxygen species (ROS), and hypoxia within the tumor microenvironment. The drawbacks of PTT include uneven temperature distribution and the upregulation of the heat-shock proteins in tumors, both of which result in ineffective treatment. To address these issues, a MnO2 doped nano-delivery system (HTIM-PMs) was synthesized by one-step self-assembly of disulfide bond bridged copolymers for indocyanine green (ICG) and MnO2 loading. The surface of polymeric micelles was layered with hyaluronan (HA) and transactivator (TAT) peptides to improve active targeting and increase cell penetration. After internalization, HTIM-PMs showed responsiveness to the tumor microenvironment (acid pH, high glutathione, high H2O2). Breaking the disulfide bond reduced the intratumoral GSH level and simultaneously released the MnO2 and ICG. The released MnO2 further reduced the GSH level and promoted O2 generation, thus enhancing the PDT effect. The PTT-mediated hyperthermia accelerated blood flow, which is beneficial for O2 distribution, and promotes ROS diffusion. These PTT-mediated adjuvant effects further overcame the limitations of PDT and the robust PDT effect in turn compensated for the deficiency of PTT. This promising platform exhibited a significant improvement in the PTT-PDT cancer treatment strategy compared to previously reported nanostructures.
Oral administration is the most acceptable route of drug delivery at this stage due to its convenience, safety, and non-invasiveness. However, drugs given orally are exposed to a complex gastrointestinal environment, causing a tremendous challenge for their successful absorption into the circulation. Over the past decades, researchers have developed various novel pharmaceutical technologies to improve oral absorption, among which the vesicular drug delivery system (like liposomes, niosomes and transfersomes) has received extensive attention. Encouragingly, there have been several investigations confirming the improved effect of vesicular drug delivery systems on oral drug absorption. Nevertheless, the clinical translation of oral vesicular drug delivery systems has been less impressive than implied by the positive results, and few vesicular formulations for oral use have been marketed yet. Against this background, this article provides an overview of the current applications and challenges associated with the vesicular delivery systems available for oral drug delivery, specifically liposomes, niosomes, transfersomes, chitosomes and bilosomes. The composition, formation mechanism, drug delivery advantages and application cases of these carriers in oral drug delivery are summarized. The possible mechanisms by which vesicular carriers enhance oral drug absorption are analyzed in terms of the in vivo process of oral drugs. Further, the challenges that oral vesicular carriers now face, such as safety, undefined in vivo fate, and scale-up production, are summarized, while possible strategies to deal with them are indicated. By reviewing the aforementioned, it can facilitate a more comprehensive knowledge of vesicular systems that can be used for oral drug delivery, providing a theoretical basis and reference for the design of oral formulations.
Due to the advantages of renewable, low pollution and wide distribution of biomass resources, it is selected as the electrode material for supercapacitors. For carbon-based electrode materials, specific surface area and pore structure have a great influence. Exploring and summarizing the influence of activation on pore structure will greatly broaden this field. Based on the activation mechanism of activator, this paper summarizes the latest progress of biomass activation applied to supercapacitors, including traditional physical and chemical activation methods and non-traditional methods such as biological activation method, self-activation method, template assisted activation method and green activator activation. Finally, the challenges, strategies and prospects for the future development of biomass-derived carbon material activation are pointed out. In summary, this review will help researchers choose appropriate strategies to design biomass-derived carbon electrode materials for supercapacitors, thereby promoting the application of biomass materials.
Rationally designed novel cost-effective hydrogen evolution reaction (HER) electrocatalysts with controlled surface composition and advanced structural superiority is extremely critical to optimize the HER performance. Polyoxometalates (POMs) with structural diversity and adjustable element compositions represent a promising precursor for rational design and preparation of HER electrocatalysts. Herein, a series of transition metal-doped MoS2 materials with different surface engineered structures (Fe, Cr, V doping and S vacancies) (M-MoS2/CC, M = Fe, Cr and V) were fabricated by a simple hydrothermal-vulcanization strategy using Keplerate polyoxomolybdate nanoball ({Mo72Fe30}, {Mo72Cr30}, {Mo72V30}, {Mo132}) as precursors. The enlarged interlayer spacing as well as the integration of homogeneous transition metal doping and abundant sulfur vacancies endows prepared M-MoS2/CC with superior HER electrocatalytic performance and excellent long-term working stability in both acidic and alkaline media. The optimized Fe-MoS2/CC afford current densities of 10 and 50 mA/cm2 at overpotentials of 188/272 mV and 194/394 mV in 0.5 mol/L H2SO4 and 1.0 mol/L KOH aqueous solution, respectively, outperforming most of reported typical transition metal sulfide-based catalysts. This work represents an important breakthrough for POMs-mediated highly efficient transition metal sulfide-based HER electrocatalysts with wide range pH activity and may provide new options for the rational design of promising HER electrocatalysts and beyond.
Herein, we unveil the intelligent detection of multiple catechol isomers in complex environments utilizing both laser-induced graphene (LIG) and artificial neural network (ANN). The large scale-up manufacturing of LIG-based sensors (LIGS) with three-electrode configuration on polyimide (PI) is achieved by direct laser-writing and screen-printing technologies. Our LIGS shows excellent electrochemical performance toward catechol isomers, i.e., hydroquinone (1, 4-dihydroxybenzene, HQ), catechol (1, 2-dihydroxybenzene, CT), and resorcinol (1, 3-dihydroxybenzene, RC), with a low limit of detection (LOD) (CC, 0.079 µmol/L; HQ, 0.093 µmol/L; RC, 1.18 µmol/L). Moreover, the ANN model is developed for machine-intelligent to predict concentrations of catechol isomers under an interfering environment via a single LIGS. Using six unique parameters extracted from the differential pulse voltammetry (DPV) response, the machine learning-based regression provides a coefficient of correlation with 0.998 and is able to correctly predict the total and individual concentrations in complex river samples. Hence, this work provides a guide for the preparation and application of LIGS via facile and cost-efficient mass production and the development of an intelligent sensing platform based on the ANN model.
Four new cyclohexapeptides, pyridapeptides F–I (1–4), were isolated from the fermentation broth of marine sponge-derived Streptomyces sp. OUCMDZ-4539. The pyridapeptides F–H (1–3) are composed of β-hydroxyleucine, alanine, O-methylthreonine, hexahydropyridazine-3-carboxylic acid, 5-hydroxytetrahydropyridazine-3-carboxylic acid, and (2S,3R,4E,6E)-2-amino-3–hydroxy-4,6-dienoic acid residues. Pyridapeptide Ⅰ (4) contains (2S,3R,4E,6E)-2-amino-3–hydroxy-8-methylnona-4,6-dienoic acid residue and a very rare glycose residue, aculose. Their structures were determined based on spectroscopic analysis and chemical methods. Pyridapeptides G–I (2–4) have the 2,3,6-trideoxyhexose units glycosylated at the γ-OH-TPDA residue, displayed significant antiproliferative activity against four (PC9, MKN45, HepG2, K562) or two (PC9, MKN45) human cancer cell lines.
The preparation of Pd-based catalysts with rich electrons and a high atom dispersion rate is of great significance for improving the reactivity of cross-coupling reactions, which is a powerful tool for pharmaceutical and fine chemical synthesis. Here, we report a PdNi single-atom alloy (SAA) catalyst in which isolated Pd single atoms are anchored onto the surface of Ni nanoparticles (NPs) applied for Suzuki coupling reactions and Heck coupling reactions. The 0.1% PdNi SAA exhibits extraordinary catalytic activity (reaction rate: 17,032.25 mmol h−1 gPd−1) toward the Suzuki cross-coupling reaction between 4-bromoanisole and phenylboronic acid at 80℃ for 1 h. The excellent activity is supposed to attribute to the 100 percent utilization rate of Pd atoms and the highly stable surface zero-valance Pd atoms, which provides abundant sites and electrons for the adsorption and fracture of the C-X (X = Cl, Br, I) bond. Moreover, our work demonstrates the excellent application prospect of SAAs for cross-coupling reactions.
To overcome the conflict between the long-wavelength excitation and high singlet oxygen quantum yield of photosensitizers, we conjugated a two-photon fluorophore, tetrahydroquinoxaline coumarin (TQ), and an efficient photodynamic therapeutic agent, benzo[a]phenothiazinium (NBS-NH2), through a hexamethylene linker to build a two-photon photosensitizer, TQ-NBS. In TQ-NBS, TQ served as an energy donor and NBS-NH2 acted as an energy acceptor; and TQ-NBS was a Förster resonance energy transfer (FRET) cassette with a 92.8% efficiency. The large two-photon absorption cross-section of TQ allowed photosensitizer TQ-NBS to work in a 900 nm two-photon excitation (TPE) mode, which greatly benefited the deep tissue penetration in PDT treatment. Meanwhile, the excellent phototoxicity and near-infrared fluorescence of NBS-NH2 was kept in TQ-NBS under a TPE mode via a FRET process. Photosensitizer TQ-NBS exhibited a high phototoxic efficacy in living cells and tumor-bearing mice.
Anticancer platinum prodrugs that can be controllably activated are highly desired for personalized precision medicine and patient compliance in cancer therapy. However, the clinical application of platinum(Ⅳ) prodrugs (Pt(Ⅳ)) is restricted by tissue penetration of external irradiation. Here, we report a novel Pt(Ⅳ) activation strategy based on endogenous luminescence of tumor microenvironment responsiveness, which completely circumvents the limitation of external irradiation. The designed Pt(Ⅳ)Lu, a mixture of trans, trans, trans-[Pt(N3)2(OH)2(py)2] and luminol (Lu), has controllable activation property: it remains inert in reductant environment and normal tissues, but under tumor microenvironment, Lu will be oxidized to produce blue luminescence, which rapidly reduce Pt(Ⅳ) to Pt(Ⅱ) without the need of any external activator. Pt(Ⅳ)Lu shows excellent responsive antitumor ability both in vitro and in vivo. Compared to cisplatin, the median lethal dose in BALB/c mice increased by an order of magnitude. Our results suggest that Pt(Ⅳ)Lu exhibits highly controllable activation property, superior antitumor activity, and good biosafety, which may provide a novel strategy for the design of platinum prodrugs.
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