Latest ArticlesThe properties of layered double hydroxides (LDHs), including the adjustability of cations in host layers, exchangeability of anions between layers, and tunability of the crystal structure, render them unique characteristics in preparation and applications. Relating to the structural characteristics of LDHs, this work analyzes the research status, advantages and disadvantages of the synthetic methods for LDHs, including hydrothermal, electrodeposition, co-precipitation and anion exchange methods. In addition, the application status and prospects are reviewed, such as photo/electrocatalysis, electrochemical energy storage, magnetic materials, pollutant adsorption, and other fields. Lastly, the critical issues and solutions in the developing process of LDHs are analyzed and proposed.
Real-time exploring the cellular endocytic pathway of viral capsid proteins (VCPs) functionalized nanocargos at the single-particle level can provide deep insight into the kinetic information involved in virus infection. In this work, porcine circovirus type 2 (PCV2) VCPs with different functions are modified onto the surface of upconversion nanoparticles (VCPs-UCNPs) to investigate the cellular internalization process in real-time. Clathrin-mediated endocytosis is found to be the essential uptake mechanism for these VCPs-UCNPs. Besides, it is verified that P1-UCNPs (PCV2 VCPs with nuclear localization signal, namely P1) can be easily assembled close to the perinuclear area, which is different from that of P2-UCNPs (PCV2 VCPs without nuclear localization signal, namely P2). Interestingly, multistep entry processes are observed. Particularly, confined diffusion is observed during the transmembrane process. The intracellular transport of VCPs-UCNPs is dependent on microtubules toward the cell interior. During this process, P1-UCNPs display increased velocities with active transport, while diffusion much faster around the perinuclear area. But for P2-UCNPs, there are only two phases involved in their endocytosis process. This study presents distinct dynamic mechanisms for the nanocargos with different functions, which would make a useful contribution to the development of robust drug delivery systems.
Solid-state batteries with high energy density and safety are promising next-generation battery systems. However, lithium oxide and lithium sulfide electrolytes suffer low ionic conductivity and poor electrochemical stability, respectively. Lithium halide solid electrolyte shows high conductivity and good compatibility with the pristine high-voltage cathode but limited applications due to the high price of rare metal. Zr-based lithium halides with low cost and high stability possess great potential. Herein, a small amount of In3+ is introduced in Li2ZrCl6 to synthesize Li2.25Zr0.75In0.25Cl6 electrolytes with a high room temperature Li-ion conductivity of 1.08 mS/cm. Solid-state batteries using Li2.25Zr0.75In0.25Cl6/Li5.5PS4.5Cl1.5 bilayer solid electrolytes combined with Li-In anode and pristine LiNi0.7Mn0.2Co0.1O2 cathode deliver high initial discharge capacities under different cut-off voltages. This work provides an effective strategy for enhancing the conductivity of Li2ZrCl6 electrolytes, promoting their applications in solid-state batteries.
Semiconductor photocatalysis holds great promise for breaking the inert chemical bonds under mild condition; however, the photoexcitation-induced modulation mechanism has not been well understood at the atomic level. Herein, by performing the DFT+U calculations, we quantitatively compare H2 activation on rutile TiO2(110) under thermo- versus photo-catalytic condition. It is found that H2 dissociation prefers to occur via the heterolytic cleavage mode in thermocatalysis, but changes to the homolytic cleavage mode and gets evidently promoted in the presence of photoexcited hole (h+). The origin can be ascribed to the generation of highly oxidative lattice O-radical (Obr·-) with a localized unoccupied O-2p state. More importantly, we identify that this photo-induced promotion effect can be practicable to another kind of important chemical bond, i.e., C–H bond in light hydrocarbons including alkane, alkene and aromatics; an exception is the C(sp1)-H in alkyne (HC≡CH), which encounters inhibition effect from photoexcitation. By quantitative analysis, the origins behind these results are attributed to the interplay between two factors: C-H bond energy (Ebond) and the acidity. Owing to the relatively high Ebond and acidity, it favors the C(sp1)-H bond to proceed with the heterolytic cleavage mode in both thermo- and photo-catalysis, and the photoexcited Obr·- is adverse to receiving the transferred proton. By contrast, for the other hydrocarbons with moderate/low Ebond, the Obr·- would enable to change their activation mode to a more favored homolytic one and evidently decrease the C–H activation barrier. This work may provide a general picture for understanding the photocatalytic R–H (R = H, C) bond activation over the semiconductor catalyst.
Ground-level ozone is one of the primary pollutants detrimental to human health and ecosystems. Catalytic ozone decomposition still suffers from low efficiency and unsatisfactory stability. In this work, we report a manganese-based layered double hydroxide catalyst (Co3Mn-LDH), which exhibited a superior ozone decomposition performance with the efficiency of 100% and stability over 7 h under a GHSV of 2,000,000 mL g-1h-1 and relative humidity of 15%. Even when the relative humidity increased to 50%, the ozone decomposition also reached 86%, which significantly exceeds as-synthesized MnO2 and commercial MnO2 in performance. The catalytic mechanism was studied by H2-TPR, FT-IR and XPS. The excellent performance of Co3Mn-LDH can be attributed to its abundant surface hydroxyl groups that ensured the preferentially surface enrichment of ozone, as well as the cyclic dynamic replenishment of electrons between multivalent Co2+/Co3+, Mn2+/Mn3+/Mn4+ and oxygen species that endowed the stable ozone decomposition. This work offers new insights into the design of efficient catalysts for ozone pollution control.
In recent years, with the emergence of new pollutants, the effective treatment of wastewater has become very important. Persulfate-based advanced oxidation processes have been successfully applied to the treatment of wastewater, such as wastewater containing antibiotics, pharmaceuticals and personal care products, dyes, endocrine-disrupting chemicals, chlorinated organic pollutants, and phenolics, for the degradation of refractory organic contaminants. This paper summarizes the production of sulfate radicals, which can be generated by the activation of persulfate via conventional and emerging approaches. The existing problems of persulfate-based advanced oxidation processes were analyzed in detail, including residual sulfates, coexisting factors (coexisting inorganic anions and natural organic matter), and energy consumption. This paper proposes corresponding possible solutions to the problems mentioned above, and this paper could provide a reference for the application of persulfate-based advanced oxidation processes in actual wastewater treatment.
Fluoroalkyl-containing organic compounds have exhibited wide applications in the field of pharmaceuticals, agrochemicals and materials science due to their outstanding properties such as biological activity, metabolic stability, lipophilicity, excellent chemical and thermal stability. Therefore, various synthetic strategies have been developed for the construction of fluoroalkyl-containing compounds, using highly active fluorinating reagents and fluorinated building blocks. Recently, the use of easily available and inexpensive trifluoroacetic anhydride (TFAA) and its anhydride analogues has attracted great attention to access numerous fluoroalkyl-containing compounds through cyclization and coupling reactions. In this review, we summarized the recent advances in the synthesis of fluoroalkylated compounds using fluoroalkyl anhydrides as reagents. This review aims to provide a reference for researchers on how to develop new synthetic straregies of fluorine-containing organic compounds and achieve kilograms or even tons preparation of fluorine-containing organic compounds using fluoroalkyl anhydrides.
Black phosphorus (BP) has attracted an ever-growing interest due to its unique anisotropic two-dimensional structure, impressive photoelectronic properties and attractive application potential. However, the tools for bandgap engineering and passivation via covalent modification of BP nanosheets remain limited to diazonium salt and nucleophilic addition methods, so that developing new modification strategies for BP nanosheets is crucial to explore its physical and chemical properties and enrich the toolbox for functionalization. Herein, we report the covalent modification of liquid-phase exfoliated BP nanosheets based on a rational analysis of BP structure. The modification of BP is achieved via carbene, a highly reactive organic mediate. The carbene modification improves the solubility and stability of BP nanosheets. Detailed microscopic and spectroscopic characterizations including infrared spectra, Raman spectra, X-ray photoelectron spectra, SEM and TEM were conducted to provide insights for the reaction. The proof of the existence of covalent bonds between BP nanosheets and organic moieties confirms the successful modification. Moreover, theoretical calculations were conducted to unveil the reaction mechanism of the two different types of bonds and the chemical property of two-dimensional BP.
A novel and efficient copper-catalyzed decarboxylative alkynylselenation of indoles with Se powder and propiolic acids has been developed. The outstanding advantages of this protocol not only nicely avoid the use of prefabricated arylselenation reagent and address the facile over-selention issues, but also enrich the chemistry of selenium powder. Importantly, this reaction could be extended to pyrrole, and the practical utility of this transformation has been demonstrated in gram-scale synthesis and late-stage indolylselenation of Clofibrate-derived propiolic acid.
A metal-free porphyrin covalent organic framework was employed as the heterogeneous photocatalyst for the synthesis of tetrahydroquinolines under aerobic conditions. With visible light irradiation of a catalytic amount of H2P-Bph-COF at room temperature, various substituted N, N-dimethylanilines and N-aryl maleimides were transformed to tetrahydroquinoline derivatives in moderate to good yields. This was the first example of the synthesis of tetrahydroquinolines via the photocatalytic aerobic annulation reaction employing the metal-free COF as the heterogeneous photocatalyst.
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