Latest ArticlesThe 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.
Electrochemical 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.
Constructing composited electrode material is considered to be an efficient strategy to improve their electrochemical performance. It can accelerate the charge transfer speed of ions and enhance the conductivity of electrode. Meanwhile, the formation of the hybrid structure can largely avoid the aggregation of two dimensional materials and increase the electrochemical active area of the electrode. In this work, we synthesize NiMoSSe electrode materials on nickel foam by a facile hydrothermal avenue. The prepared composite shows a specific capacitance of 1035 C/g at 1 A/g due to the synergistic effect between MoS2 and MoSe2 phases. In addition, the devices are assembled with NiMoSSe samples, which offers an energy density of 82.71 Wh/kg at a power density of 2700 W/kg.
With the increasing emergence of bacterial infections, especially multidrug-resistant (MDR) bacteria, poses an urgent threat. This study demonstrated a novel multifunctional nanotheranostics platform developed by the strategic integration of both in-situ bio-assembly imaging and target bacteria inactivation. Through the introduction of copper ions into bacteria, the Cu2+ could spontaneously bio-self-assembled into a multifunctional copper nanoclusters (NCs) which efficiently enhanced epigallocatechin gallate (EGCG) uptake into bacteria. While visualizing the bacteria, the developed theranostic nanoplatform exhibited highly efficient disinfection activities with negligible side effects as reflected by higher cell viability and insignificant hemolytic effects. Furthermore, the exosomal formulation of EGCG integrated with Cu2+ showed an increased intracellular antibacterial activity, which could eliminate most of the methicillin-resistant Staphylococcus aureus (MRSA) phagocytosed by macrophages, guide macrophages toward M2-like phenotype polarization and alleviate inflammation, without exhibiting obvious cytotoxicity on host RAW264.7. The regimen could be viewed as an effective strategy for the sterilization of intractable bacterial infections.
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.
Strand displacement reaction enables the construction of enzyme-free DNA reaction networks, thus has been widely applied to DNA circuit and nanotechnology. It has the characteristics of high efficiency, universality and regulatability. However, the existing regulation tools cannot enable effective control of the reaction sequence, which undoubtedly limits the construction of complex nucleic acid circuits. Herein, we developed a regulation tool, toehold lock, and achieved strict control of reaction sequence without loss of the main reaction signal output. Furthermore, we applied the tool to scenarios such as seesaw circuits, AND/OR logic gates, and entropy-driven circuits, and respectively demonstrated its significant superiority compared to the original method. We believe that the proposed toehold lock has greatly optimized the efficiency of DNA strand displacement-based networks, and we anticipate that the tool will be widely used in multiple fields.
Size is one of the most important characteristics of nanoparticles to influence their biodistribution and antitumoral efficacy. Particles with large sizes have difficulty in deep tumor penetration, while small particles are easily removed from tumor tissues due to the high tumor interstitial fluid pressure. To address these issues, an intelligent core-crosslinked polyion complex micelle (cPCM) with a reversibly size-switchable feature was engineered in this study. The micelles are consisting of methoxy poly(ethylene glycol)-poly(D,L-lactide) copolymer (mPEG-PLA), mPEG-PLA-(HE)6CC, and mPEG-PLA-(RG)6CC at an optimal mass ratio of 6:1:1 with an antiangiogenic compound, dabigatran etexilate (DE), encapsulated. The net charge inside the micelles is switchable when exposed to different pH conditions, thereby leading to revisable size-change of micelles. DE-loaded micelles (DE@cPCM) can swell and release drugs at the tumor sites with a mildly acidic pH, while they shrink and protect the cargo from leaking into the blood circulation with a neutral pH. Results indicated that DE@cPCM can inhibit tumor angiogenesis in vitro and in vivo, thereby efficiently restraining tumor growth in a 4T1-bearing mouse model. Collectively, the size-switchable cPCM is a promising nanoplatform for targeting delivery of anticarcinogens into the matrix of tumor tissues.
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.
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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