Latest ArticlesMicroplasma based on glow discharge could act as a non-contact gaseous electrode and has attracted much attention in both fundamental research and application. Herein, with microplasma as the anode, the electrodeposition process of a series of metal and metal alloys in molten salt has been systemically studied. Four metal cations with different valence states, silver (Ag+), nickel (Ni2+), copper (Cu2+), and iron (Fe3+), could all be reduced on the solid cathode with high current efficiency and the corresponding metal products were of high purity. The electrodeposition of aluminum-lanthanum (Al-Ln) alloy on the aluminum cathode was also successfully carried out with microplasma as the anode, and the same alloy was obtained by using the conventional anode electrode. These results indicated that microplasma anode based on non-contact direct-current (DC) glow discharge is a promising electrode to be applied in molten salt electrolysis.
Popularization of lithium-sulfur batteries (LSBs) is still hindered by shuttle effect and volume expansion. Herein, a new modularized sulfur storage strategy is proposed to solve above problems and accomplished via employing 100% space utilization host material of cobalt loaded carbon nanoparticles derived from ZIF-67. The modular dispersed storage of sulfur not only greatly increases the proportion of active sulfur, but also inhibits the occurrence of volume expansion. Meanwhile, 100% space utilization host material can greatly improve the conductivity of the cathode, provide a larger electrolyte wetting interface and effectively suppress the shuttle effect. Moreover, loaded cobalt particles have high catalytic activity for electrochemical reaction and can effectively improve the redox kinetics. The cell with new cathode host material carbonized at 650 ℃ (ZIF-67 (650 ℃)) exhibits superior rate performance and can maintain a high specific capacity of 950 mAh/g after 100 cycles at 0.2 C, showing a good cycle stability.
Despite the synergy of immune checkpoint blockade (ICB) therapy and photodynamic therapy (PDT) holds great promise as countermeasures against breast cancer, exploring long-term or flexible short-time therapeutic strategies in "cold" tumors remains a great challenge. Here, we present a polyunsaturated fatty acid-doped liposomal hydrogel Lp(DHA)@CP Gel loaded with photosensitizer chlorin e6 (Ce6) and programmed death-ligand 1 antibody (αPD-L1) for flexible local photoimmunotherapy with merely single-dosed administration. The presence of polyunsaturated fatty acid (docosahexaenoic acid, DHA) doped in particle membrane endows liposomes with flexibly reactive oxygen species (ROS)-responsive release capability, which was attributed to the presence of abundant unsaturated groups. The αPD-L1 was repeatedly induced to in situ release in response to the PDT under photo-exposure. The immunogenic cell death (ICD) effect of PDT evoked "cold" breast tumor to "hot" one, and then assisted the cascade released αPD-L1 to synergistically boost the immunotherapy. After a single dose of peritumoral administration of Lp(DHA)@CP Gel, the on-demand treatment can maximize patient compliance and safety by adjusting therapeutic behaviors via a photo on-off switch. This work presents a flexible medication platform, showing promise in improving the objective response rate of ICB therapy and minimizing its systemic toxicity.
LiNi0.8Co0.15Al0.05O2 (NCA) is a promising cathode for sulfide-based solid-state lithium batteries (ASSLBs) profiting from its high specific capacity and voltage plateau, which yielding high energy density. However, the inferior interfacial stability between the bare NCA and sulfides limits its electrochemical performance. Hereien, the dual-electrolyte layer is proposed to mitigate this effect and enhance the battery performances of NCA-based ASSLIBs. The Li3InCl6 wih high conductivity and excellent electrochemcial stability act both as an ion additives to promote Li-ion diffusion across the interface in the cathode and as a buffer layer between the cathode layer and the solid electrolyte layer to avoid side reactions and improve the interface stability. The corresponding battery exhibits high discharge capacities and superior cyclabilities at both room and elevated temperatures. It exhibits discharge performance of 237.04 and 216.07 mAh/g at 0.1 and 0.5 C, respectively, when cycled at 60 ℃, and sustains 95.9% of the capacity after 100 cycles at 0.5 C. The work demonstrates a simple strategy to ensure the superior performances of NCA in sulfide-based ASSLBs.
Humans have relied on biomass for survival and development since the Stone Age. All aspects of human needs for materials are covered by tools, fuel, and buildings. Nowadays, metals and petroleum-based materials are widely used in highly developed industries. Unfortunately, environmental contamination and the loss of natural resources have led to the reemergence of biomass resources as efficient and sustainable energy sources. Notably, simple and direct applications can no longer meet the demand for functionalization, high performance of materials and construction materials. Therefore, it is imperative to modify biomass and combine its utilisation to produce functionalization and high performance materials. For example, construction materials with superior mechanical properties and water resistance can be produced by reinforcing fibres to facilitate crosslinking. Water-oil separation or adsorption effects of hydrogels and aerogels are determined by the porosity and lightness of biomass, biocomposite conductor is prepared by chimaeric conductive material. Here, we review the approaches that have been taken to devise an environmentally friendly yet fully recyclable and sustainable functionalised biocomposites from biomass and its potential directions for future research.
Lipid-based nanocarriers have staged a remarkable comeback in the oral delivery of proteins and peptides, but delivery efficiency is compromised by lipolysis. β-Lactoglobulin (β-lg) stabilized lipid nanoparticles, including nanoemulsions (NE@β-lg) and nanocapsules (NC@β-lg), were developed to enhance the oral absorption of insulin by slowing down lipolysis due to the protection from β-lg. Cremophor EL stabilized nanoemulsions (NE@Cre-EL) were prepared and set as a control. The lipid nanoparticles produced mild and sustained hypoglycemic effects, amounting to oral bioavailability of 3.0% ± 0.3%, 7.0% ± 1.1%, and 7.7% ± 0.8% for NE@Cre-EL, NE@β-lg, and NC@β-lg, respectively. Aggregation-caused quenching (ACQ) probes enabled the identification of intact nanoparticles, which were used to investigate the in vivo and intracellular fates of the lipid nanoparticles. In vitro digestion/lipolysis and ex vivo imaging confirmed delayed lipolysis from β-lg stabilized lipid nanoparticles. NC@β-lg was more resistant to intestinal lipolysis than NE@β-lg due to the Ca2+-induced crosslinking. Live imaging revealed the transepithelial transport of intact nanoparticles and their accumulation in the liver. Cellular studies confirmed the uptake of intact nanoparticles. Slowing down lipolysis via food proteins represents a good strategy to enhance the oral absorption of lipid nanoparticles and thus co-formulated biomacromolecules.
In this work, we designed and synthesized cationic carbon dots (CDs) with a size distribution of 1.6–3.7 nm, which exhibited dark blue fluorescence in the aqueous solution. Based on its excellent luminescence properties, we used it as an energy donor to construct a sequential artificial light-harvesting system (LHS) by employing the energy-matching dyes eosin Y disodium salt (EY) and sulforhodamine 101 (SR101), which could regulate the white light emission (Commission Internationale de lʼEclairage (CIE) coordinate: (0.30, 0.31)) with the energy transfer efficiency (ΦET) of 53.9% and 20.0%. Moreover, a single-step artificial LHS with white light emission (0.32, 0.28) can be constructed directly using CDs and dye solvent 43 (SR) with ΦET and antenna effect (AE) of 48.8% and 6.5, respectively. More importantly, CDs-based artificial LHSs were firstly used in photocatalytic of α-bromoacetophenone, with a yield of 90%. This work not only provides a new strategy for constructing CDs-based LHSs, but also opens up a new application for further applying the energy harvested in CDs-based LHSs to the field of the aqueous solution photocatalysis.
Mg-doped manganese oxide octahedral molecular sieve (Mg-OMS-2) catalysts were prepared by hydrothermal method. The photothermal degradation performance of these catalysts for formaldehyde (HCHO) in batch system and continuous system was investigated. The light absorption of OMS-2 was increased by Mg-doped, especially for near infrared light, which promoted surface temperature reach a maximum of 214.8 ℃ under xenon irradiation. At this temperature, the reinforced surface lattice oxygen and oxygen vacancy that formed by lattice distortion via Mg-doped were activated. The best HCHO elimination efficiency was achieved over Mg0.2/OMS-2 catalyst with Mg2+/Mn2+ = 1/5, which could reduce HCHO from 250 ppm to 10 ppm within 20 min. The in situ DRIFTS was also carried out to monitor the changes in the content of reaction intermediates and analyze the degradation paths of HCHO. It was found the HCHO was attacked by formed •OH and •O2− to generate formate species and carbonate species, and finally transformed to CO2 and H2O. This photothermal catalytic oxidation process exhibited a high efficiency purification of HCHO without the help of extra energy consumption.
Modern chromatography is increasingly focused on miniaturization and integration. Compared to conventional liquid chromatography, microfluidic chip liquid chromatography (microchip-LC) has the potential due to its zero-dead volume connection and ease of integration. Nano-sized packings have the potential to significantly enhance separation performance in microchip-LC. However, their application has been hindered by packing difficulties. This study presents a method for packing nano-sized silica particles into a microchannel as the stationary phase. The microchip-LC packed column was prepared by combining the weir and the porous silica single-particle as frit to retain the packing particles. A surface tension-based single-particle picking technique was established to insert porous single-particle frit into glass microchannels. Additionally, we developed a slurry packing method that utilizes air pressure to inject nano-sized packing into the microchannel. Pressure-driven chromatographic separation was performed using this nano-packed column integrated into a glass microchip. The mixture of four PAHs was successfully separated within just 8 min using a 5 mm separation channel length, achieving high theoretical plates (106 plates/m). Overall, these findings demonstrate the potential of utilizing nano-sized packings for enhancing chromatographic performance in microchip systems.
Due to the high electrophilic nature of azo-dienophiles, azo-Diels–Alder proceeds rapidly even without the need of a catalyst and is therefore regarded as the "click reaction". This spontaneity causes strong background reaction and poses a daunting challenge to chemists for developing the catalytic asymmetric version. Reported herein is the first catalytic asymmetric dearomative azo-Diels–Alder reaction between 2-vinylindoles and triazoledione. This protocol makes use of the high energy barrier of dearomatization to avert the strong background reaction of azo-Diels–Alder reaction, allowing the implementation of the projected reaction at ambient temperature. Density functional theory calculations have been performed to gain insights into the reaction mechanism and the origins of the enantioselectivity. By using this method, a variety of tetracyclic indole derivatives have been readily prepared in good to excellent yields and with excellent diastereo- and enantio-selectivities (33 examples, up to 97% yield and > 99% ee, > 20:1 dr).
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