Achieving high energy densities for all-solid-state lithium batteries is restricted by the poor high voltage stability of solid electrolytes. Herein, F-doping strategy is successfully employed on Li3InCl6 to obtain enhanced voltage stability and electrode compatability towards bare LiNi0.7Mn0.2Co0.1O2 at high voltages. The optimized Li3InCl5.5F0.5 electrolyte exhibits a decreased conductivity of 1.00 mS/cm, a wider voltage window, and improved electrochemical performance in solid-state batteries when cycled at upper cut-off voltages of 4.5 and 4.8 V (vs. Li+/Li0). The generation of more stable LiInF4 phase in the cathode mixture of Li3InCl5.5F0.5-based battery ensures superior electrochemical performances compared to the Li3InCl6-based battery. The former battery exhibits a higher discharge capacity of 218.9 mAh/g and coulombic efficiency of 86.7% for the first cycle, and retains 80.0% of its original value after 100 cycles when cycled in the range of 3.0–4.5 V (vs. Li+/Li0). In contrast, the Li3InCl6-based battery exhibits lower capacities and faster degradation under the same conditions due to the formation of InCl3 phase with poor electrochemical stability. This work facilitates the advancement of high energy density solid-state battery technologies by utilizing high-voltage cathodes.
Mitochondria are crucial organelles responsible for maintaining cell growth, and their homeostasis is closely linked to pH regulation. Physiologically, mitochondria exhibit a weakly alkaline state (pH~8.0). However, when subjected to stress stimuli that cause damage, cells initiate the process of mitophagy, resulting in mitochondrial acidification. Therefore, monitoring changes in mitochondrial pH to comprehend the physiological processes associated with mitophagy is essential. In this study, we developed an asymmetric pentamethine cyanine dye Cy5.5-H-CyN as a probe for continuous monitoring of mitophagy in living cells. By incorporating an azaindole structure into the dye molecule, a ratiometric fluorescence response was achieved that is specifically responsive to pH variations while preserving its ability to target mitochondria and emit near-infrared fluorescence. Through various methods inducing mitophagy, Cy5.5-H-CyN was employed to determine mitochondrial pH quantitatively, demonstrating its suitability as an ideal probe for continuous monitoring of mitophagy in living cells.
Boron-doped diamond (BDD) is a well-known anode material with a high pollutant degradation ability for electrochemical oxidation wastewater treatment. Nevertheless, the cost of production and mechanical strength of BDD membranes remain unsatisfactory. Magnetic BDD particles derived from industrial waste may represent a promising alternative to BDD membranes, although the challenge remains in assembling these particles into a usable electrode. In this study, magnetic BDD particles were attracted to a Ti/RuO2-IrO2 electrode using a magnet, thus constituting a novel 2.5-dimensional (2.5D) electrode. To ascertain the structure-activity relationship of the novel electrode, essential characterizations, multi-physics simulations, pollutant degradation and electrosynthesis experiments were conducted. The results indicate that an appropriate quantity of BDD particles (0.1 g/cm2) can enhance the number of active sites by approximately 20%. A strong synergistic effect was observed between the Ti/RuO2-IrO2 and BDD particles in the degradation of various pollutants, including azo dye, p-benzoquinone, succinic acid and four kinds of real wastewaters, as well as glycerol conversion. The joint active sites on the interface between Ti/RuO2-IrO2 and BDD particles, as well as the inner active sites on BDD particles, have been identified as crucial in the mineralization of pollutants and the generation of value-added products. The optimal amount of BDD particles (0.1 g/cm2) is sufficient to preserve the joint active sites and to maintain an adequate polarization on the BDD particles. Nevertheless, the hybrid feature of the 2.5D electrode is diminished when a greater quantity of BDD particles (0.3 g/cm2) is loaded.
2-Azabicyclo[2.1.1]hexanes (aza-BCHs) are constrained pyrrolidine analogues with improved physicochemical characteristics in drug design. Here, we report a direct visible light-mediated photocycloaddition of 4-aza-coumarins with mono- or disubstituted bicyclo[1.1.0]butanes for synthesizing aza-BCHs without an external catalyst. The introduction of the ester group on 4-azacoumarin is critical for direct imine excitation and versatile synthetic utility. Preliminary mechanistic studies indicated that the reaction took place primarily at the triplet hypersurface.
A renewable fluorescent material (G⊂CP5L) has been constructed via supramolecular assembly between a new derivative of pillararene, namely leggero pillar[5]arene, as the host molecule (CP5L) and a tetraphenylethylene (TPE)-based ditopic guest (G). This new material can simultaneously perform efficient detection and separation of silver(Ⅰ) from aqueous environments. Possessing an electron-rich cavity and two cytosine groups modified on both rims, CP5L functions as the host-guest binding site for G and offers exclusive coordination sites for further interaction with Ag+. Adding Ag+ to the system undergoes dramatic fluorescence enhancement due to the mechanism of supramolecular assembly-induced enhanced emission (SAIEE). This fluorescence enhancement allows for efficient and visualized detection following a "light-up" pattern, achieving a limit of detection (LOD) of 1.3 × 10–7 mol/L, which is fully in line with the World Health Organization's drinking water standard of 9 × 10–7 mol/L. In addition, G⊂CP5L also shows strong anti-interference capability against other cationic species. For the separation of Ag+ from aqueous systems, G⊂CP5L displays exceptional adsorption efficiency (97%) and reliable recovery performance, demonstrating excellent recyclability after five experimental cycles without compromising its adsorption activity
A novel photocatalytic energy transfer-driven radical relay strategy has been introduced for the chemo- and regioselective 1, 4-difunctionalization of carbon-sulfur double bonds. This represents the first instance of radical-mediated dual-functionalization of X-Y type unsaturated bonds, enabling the synthesis of complex linear molecules with CO, CN, and C-S bonds in a single operation. The method surpasses traditional approaches by avoiding the need for thiourea intermediates and the harsh conditions typically associated with them. The developed strategy exemplifies versatility, being applicable to 1, 4-oxyamination, 1, 4-diamination, and 1, 4-sulfonamination reactions, and has demonstrated compatibility with over 60 different substrates. The research also elucidates the role of electronic complementarity between radicals and receptors in achieving high selectivity in 1, 4-difunctionalization reactions. This study significantly advances the field of bifunctionalization and remote difunctionalization reactions, with profound implications for the development of pharmaceuticals and materials science.
Electrocatalysis for nitrate (NO3–) removal from wastewater faces the challenge of merging efficient reduction and high selectivity to nitrogen (N2) with economic viability in a durable catalyst. In this study, bimetallic PdCu/TiOx composite catalysts were synthesized with varying Pd and Cu ratios through electrochemical deposition on defective TiOx nanotube arrays. Denitrification experiments demonstrated that the Pd1Cu1/TiOx catalyst exhibited the highest NO3– removal rate (81.2%) and N2 selectivity (67.2%) among all tested catalysts. Leveraging the exceptional light-responsive property of TiOx, the introduction of light energy as an assisting factor in electrocatalysis further augmented the NO3– treatment rate, resulting in a higher NO3– removal rate of 95.1% and N2 selectivity of approximately 90%. Compared to individual electrocatalysis and photocatalysis systems, the overpotential for the catalytic interface active *H formation in the photo-assisted electrocatalysis system was remarkably reduced, thus accelerating electron migration and promoting NO3– reduction kinetics. Economic analysis revealed an energy consumption of 2.74 kWh/mol and a corresponding energy consumption per order (EEO) of 0.79 kWh/m3 for the Pd1Cu1/TiOx catalyst to reduce 25.2 mg/L of NO3–-N in water to N2, showcasing remarkable competitiveness and economic advantages over other water treatment technologies. This study developed the PdCu/TiOx electrocatalysts with high NO3– removal rates and N2 selectivity, particularly when combined with light energy, the efficiency and selectivity were significantly enhanced, offering a competitive and economically viable solution for wastewater treatment.
Quantum dots (QDs), a type of nanoscale semiconductor material with unique optical and electrical properties like adjustable emission and high photoluminescence quantum yields, are suitable for applications in optoelectronics. However, QDs are typically degraded under humid and high-temperature circumstances, greatly limiting their practical value. Coating the QD surface with an inorganic silica layer is a feasible method for improving stability and endurance in a variety of applications. This paper comprehensively reviews silica coating methodologies on QD surfaces and explores their applications in optoelectronic domains. Firstly, the paper provides mainstream silica coating approaches, which can be divided into two categories: in-situ hydrolysis of silylating reagents on QD surfaces and template techniques for encapsulation QDs. Subsequently, the recent applications of the silica-coated QDs on optoelectronic fields including light-emitting diodes, solar cells, photodetectors were discussed. Finally, it reviews recent advances in silica-coated QD technology and prospects for future applications.
Multi-metal porous crystalline materials (MPCM), integrating the functions of both multi-metal centres and porous crystalline materials (e.g., metal-organic frameworks (MOFs) and covalent organic frameworks (COFs)), are an extended class of porous materials that have attracted much attention for a broad range of applications. Owing to the advantages of these materials, they generally display high porosity, multi-metal active sites, well-tuned functions, and pre-designable structures, etc., serving as desired platforms for the study of structure-property relationships. In view of the clean and sustainable target, a series of MPCM have been explored as electrocatalysts for electrocatalytic reactions like hydrogen evolution reaction, oxygen evolution reaction and electrocatalytic CO2 reduction reaction. Concerning the progress achieved for MPCM in electrocatalytic field during past years, this review will provide a brief introduction on the recent breakthrough of MPCM based electrocatalysts including their synthesis methods, structure design, component/morphology tuning, electrocatalytic property and structure-property relationship, etc. Besides, it will also conclude the current challenges and present perspectives for the MPCM based electrocatalysts, which might promote the development of porous crystalline materials in electrocatalysis and hope to provide new insights for scientists in related fields.