Latest ArticlesElectrochemical CO reduction (ECOR) as a potential strategy for producing valuable chemicals and fuels has captured substantial attention. However, the currently available electrocatalysts suffer from poor selectivity and low Faradaic efficiency, limiting their industrial application. Herein, we systematically investigate the potential of homonuclear bimetallic electrocatalysts, TM2@C9N4 (TM = Fe, Co, Ni, and Cu), for the ECOR through extensive density functional theory calculations. Our findings suggest that all four proposed monolayers exhibit exceptional stability, making them highly suitable for experimental synthesis and practical applications. Interestingly, these transition-metal dual atoms anchored on C9N4 monolayers show great potential in facilitating the production of high-value C2 products, such as C2H5OH and C2H4, due to the significantly low limiting potentials (-0.06~-0.46 V) and small kinetic energy barriers (0.54–1.08 eV) for the CO coupling process. Moreover, with the exception of Ni2@C9N4, these bimetallic catalysts demonstrate the impressive suppression of the competitive hydrogen evolution reaction (HER), leading to a high selectivity for C2 products in ECOR. Our predictions would accelerate the development of high-performance C9N4-based dual-atom catalysts for the ECOR.
The steep reduction in costs and systematic optimization of renewable electricity has ignited an intensifying interest in harnessing electroreduction of carbon dioxide (CO2RR) for the generation of chemicals and fuels. The focus of research over the past few decades has been on the optimization of the electrode and the electrolyte environment. Notably, cation species in the latter have recently been found to dramatically alter the selectivity of CO2RR and even their catalytic activity by multiple orders of magnitude. As a result, the selection of cations is a critical factor in designing catalytic interfaces with high selectivity and efficiency for targeted products. Informed decision-making regarding cation selection relies on a comprehensive understanding of prevailing electrolyte effect models that have been used to elucidate observed experimental trends. In this perspective, we review the hypotheses that explain how electrolyte cations influence CO2RR by mechanisms such as through tuning of the interfacial electric field, buffering of the local pH, stabilization of the key intermediates and regulation of the interfacial water. Our endeavor is to elucidate the molecular mechanisms underpinning cation effects, thus fostering the evolution of more holistic and universally applicable predictive models. In this regard, we highlight the current challenges in this area of research, while also identifying potential avenues for future investigations.
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.
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.
Indole is a biologically active compound formed by the fusion of benzene and pyrrole, and it is widely found in natural products and drugs. Due to the unique structure and properties of indole, its derivatives often exhibit distinctive physiological activities, which has led to widespread attention in the field of pesticide development. Analyzing the design strategies and structure-activity relationships (SARs) of compounds is a crucial step in developing novel pesticides. This review mainly summarizes indole compounds with plant growth regulating, antiviral, fungicidal, herbicidal, and insecticidal activities, with the aim of providing new insights into the discovery and mechanism of action of novel indole-based pesticides.
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.
The rapid development of high-power and pulsed-power techniques inspires extensive investigates on high-performance ceramic-based capacitors. However, the low recoverable energy density (Wrec) hampers their wider applications. Herein, the non-stoichiometric Bi0.5Na0.5TiO3-based ceramics were designed and studied. The proper introduction of oxygen vacancies facilitated activating defect dipole, giving rise to reduced remanent polarization. Consequently, the optimal composition exhibited an exceptional high Wrec of 8.3 J/cm3, a high efficiency of 85%, and excellent anti-fatigue and thermal reliability. This work provides an efficient approach to explore ceramic capacitors with high capacitive energy storage performances.
This research aims to develop a non-invasive strategy for small interfering RNA (siRNA) nasal delivery based on ionic liquids (ILs) and cationic lipid (2,3-dioleoyloxy-propyl)-trimethylammonium-chloride (DOTAP). Other than the classical role of penetration enhancer, ILs also acted as superior solvents to simultaneously load siRNA and DOTAP, forming siRNA-DOTAP-ILs (siRNA-DILs) formulations. During nasal mucosa penetration, DOTAP and ILs components self-assembled into cationic lipid nanocomplexes to load siRNA for enhanced in situ transfection. The siRNA-DILs demonstrated resistance against RNase, significant mucosa penetration, prolonged nasal retention, and satisfying gene-silencing efficacy at lower dosage. Meanwhile, DILs were also able to deliver KCa3.1-targeted siRNA effectively for the treatment of allergic rhinitis in rat model by nasal route. Thus, DILs have great potentials to deliver biological macromolecules across nasal mucosa by in situ dynamic self-assembly.
Benzene series as highly toxic gases have inevitably entered human life and produce great threat to human health and ecological environment, and thus it is distinctly meaningful to monitor benzene series with quickly, real-time and efficient technique. Herein, novel sulfur-doped mesoporous WO3 materials were synthesized via classical in-situ solvent evaporation induced co-assembly strategy combined with doping engineering, which possessed highly crystallized frameworks, high specific surface area (40.9–63.8 m2/g) and uniform pore size (~18 nm). Benefitting from abundant oxygen vacancy and defects via S-doping, the tailored mesoporous S/mWO3 exhibited excellent benzene sensing performance, including high sensitivity (50 ppm vs. 48), low detection limit (ca. 500 ppb), outstanding selectivity and favorable stability. In addition, the reduction of band gap resulted from S-doping promotes the carrier migration in the sensing materials and the reaction at the gas–solid sensing interfaces. It provides brand-new approach to design sensitive materials with multiple reaction sites.
Mercury ion (Hg2+), as one of the most toxic heavy metal ions, accumulates easily in the environment, which can generate potential hazards to the ecosystem and human health. To effectively detect and remove Hg2+, we fabricated four types of carbon dots (CDs) using carboxymethyl nanocellulose as a carbon source doped with different elements using a hydrothermal method. All the CDs exhibited a strong fluorescence emission, excitation-dependent emission and possessed good water dispersibility. Moreover, the four fluorescent CDs were used for Hg2+ recognition in aqueous solution, where the CDs-N exhibited better sensitivity and selectivity for Hg2+ detection, with a low limit of detection of 8.29 × 10−6 mol/L. It was determined that the fluorescence quenching could be ascribed to a photoinduced charge-transfer processes between Hg2+ and the CDs. In addition, the CDs-N were used as a smart invisible ink for anti-counterfeiting, information encryption and decryption. Furthermore, the CDs-N were immersed into a cellulose (CMC)-based hydrogel network to prepare fluorescent hydrogels capable of simultaneously detecting and adsorbing Hg2+. We anticipate that this research will open possibilities for a green method to synthesize fluorescent CDs for metal ion detection and fluorescent ink production.
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