Latest ArticlesA facile synthesis of 1,3,4-oxadiazoles and 1,3,4-oxadiazoles-d5 via [4 + 1] cyclization of ClCF2COONa with non-amine compounds containing amino groups is developed. Of note, this is the first time that halofluorinated compounds are used as C1 synthon to construct deuterated nitrogen-heterocyclic compounds. The current protocol features simple operation, readily accessible raw materials, wide substrate scope and valuable products
Since the outer surface interaction of Q[n]s (OSIQ, including self-, anion- and aromatic-induced OSIQs) was proposed in 2014, it has become the most important research area in our group to construct various Q[n]-based supramolecular frameworks via the OSIQ strategy. Herein, we report a novel supramolecular framework constructed using cucurbit[8]uril (Q[8]) and 4-sulfocalix[6]arene (SC[6]A). This Q[8]/SC[6]A-based supramolecular framework is a product via the perfect combination of self-, anion- and aromatic-induced OSIQs. This framework has the characteristics of easy preparation and high stability with the most important feature being the sequence selective capture of specific metal cations, such as common alkali- and alkaline earth metal ions, and renewability. Thus, this framework may be used in seawater desalination, potassium ion enrichment, radioactive cesium ion pollution source treatment, Gruinard's treatment or water softening and other applications.
Formic acid (FA), which can be produced via CO2 reduction and biomass conversion, has received extensive interest as a convenient and safe hydrogen carrier due to its wide range of sources, renewable, high hydrogen content (4.4 wt%), and convenient storage/transportation. Designing highly efficient catalysts is the main challenge to realize the hydrogen production from FA. In this work, well-dispersed and electron-rich PdIr alloy nanoparticles with a size of 1.8 nm are confined in amino-modified 3D mesoporous silica KIT-6 and applied as a highly efficient catalyst for robust hydrogen production from FA at ambient temperature. Small PdIr alloy nanoparticles confined by amino-modified KIT-6 (PdIr/KIT-6-NH2) lead to better catalytic activity compared to that of Pd/KIT-6-NH2 and PdIr confined by bare KIT-6, achieving a high turnover frequency (TOF) value of 3533 h−1 at ambient temperature (303 K), 100% H2 selectivity and conversion toward the dehydrogenation of FA, which is comparable to the best heterogeneous catalysts ever reported. The high catalytic activity of PdIr/KIT-6-NH2 can be attributed to the synergistic effect between Pd and Ir, strong interaction between PdIr and KIT-6-NH2, as well as the amino-groups of KIT-6-NH2 which can act as a proton scavenger to promote the breaking of O-H bond of formic acid.
Molecules with multifunctional properties are of immense interest in hybrid materials, while challenges still existed because of the limited compatibility of multiple functionalities in a single system. In this work, a series of metal-organic complexes were synthesized and characterized under the assembly of electron donor phosphonate, electron acceptor polypyridine ligand and spin carrier rare earth ions. All the compounds exhibited remarkable and reversible responses with photochromism and photomodulated fluorescence, originated from photogenerated radicals via electron transfer from phosphonates to polypyridine ligands. For the Dy analog, slow magnetic relaxation was observed at cryogenic temperature, indicating the single-molecule magnetic behavior. Furthermore, photogenerated radicals could enhance the proton conductive behavior, with about 2 times larger in magnitude after light irradiation for Dy and Y compounds. The introduction of photoluminescence, magnetism and proton conduction into metallic phosphonates can provide potential applications for photochromic materials.
All-inorganic CsPbI2Br perovskite with suitable bandgap and excellent thermal stability has been reported as the most promising candidate for efficient perovskite solar cells (PSCs). However, the high annealing temperature (> 250 ℃) and poor stability of α-CsPbI2Br greatly limit the future application in photovoltaic field. Herein, a facile method is reported to prepare α-CsPbI2Br perovskite film with high stability at low temperature (70 ℃) by incorporating a small amount of γ-aminobutyric acid (GABA) in the precursor solutions. The devices exhibit reproducible photovoltaic performance with a champion efficiency up to 15.16%, along with the excellent stability, maintaining more than 80% of its initial efficiency after stored in ambient condition for 600 h without any encapsulation. Most importantly, the method enables fabrication of semitransparent CsPbI2Br PSCs with a PCE of 6.76%, as well as an average visible transparency (AVT) of 25.38%. To the best of our knowledge, this is the first attempt to apply CsPbI2Br to the semitransparent solar cells.
An inexpensive Fe doped aluminoborate consisted of 18% Fe in PKU-1 material that exhibits high selectivity of 4-hydroxymethy-2,2-dimethyl-1,3-dioxolane (Solketal, 98.3%), considerable activity (TOF 51.7 h-1), and recyclable ability in the ketalization of glycerol to Solketal with acetone at 318 K has been developed. Our study demonstrated that the structure of Fe (less agglomerated iron species vs. FeOx clusters) can be tuned by changing Fe loading in the PKU-1 material, which correlated well with experimental observations. Furthermore, the surface boron sites were promoted by iron loading and behaved as Lewis-acid sites to facilitate the reaction process of glycerol ketalization, while the Solketal selectivity was closely related with the structure of iron species in PKU-1, which was proved by kinetic studies, density function theory (DFT) calculations, and a series of spectroscopy studies. This investigation demonstrates that the surface B sites can play important roles in the reaction instead of being spectators.
Sodium-ion batteries (SIBs) are promising alternatives to lithium-ion batteries (LIBs) for large-scale energy storage considering the abundance and low cost of Na-containing resources. However, the energy density of SIBs has been limited by the typically low specific capacities of traditional intercalation-based cathodes. Metal fluorides, in contrast, can deliver much higher capacities based on multi-electron conversion reactions. Among metal fluorides, CuF2 presents a theoretical specific capacity as high as 528 mAh/g while its Na-ion storage mechanism has been rarely reported. Here, we report CuF2 as a SIB cathode, which delivers a high capacity of 502 mAh/g but suffers from poor electrochemical reversibility. As a solution, we adjust the cell configuration by inserting a carbon-coated separator, which hinders the transportation of dissolved Cu ions and improves the reversibility of the CuF2 cathode. By using in-situ XRD measurements and theoretical calculation, we propose that a one-step conversion reaction occurs during the discharge process, and a reconversion reaction competes with the oxidization of Cu to dissolved Cu ion during the charge process.
Localized surface plasmon resonance (LSPR) enhanced photocatalysis has fascinated much interest and considerable efforts have been devoted toward the development of plasmonic photocatalysts. In the past decades, noble metal nanoparticles (Au and Ag) with LSPR feature have found wide applications in solar energy conversion. Numerous metal-based photocatalysts have been proposed including metal/semiconductor heterostructures and plasmonic bimetallic or multimetallic nanostructures. However, high cost and scarce reserve of noble metals largely limit their further practical use, which drives the focus gradually shift to low-cost and abundant nonmetallic nanostructures. Recently, various heavily doped semiconductors (such as WO3-x, MoO3-x, Cu2-xS, TiN) have emerged as potential alternatives to costly noble metals for efficient photocatalysis due to their strong LSPR property in visible-near infrared region. This review starts with a brief introduction to LSPR property and LSPR-enhanced photocatalysis, the following highlights recent advances of plasmonic photocatalysts from noble metal to semiconductor-based plasmonic nanostructures. Their synthesis methods and promising applicability in plasmon-driven photocatalytic reactions such as water splitting, CO2 reduction and pollution decomposition are also summarized in details. This review is expected to give guidelines for exploring more efficient plasmonic systems and provide a perspective on development of plasmonic photocatalysis.
Because the widely used perfluorooctane sulfonate (PFOS) is harmful to both environment and human health, it is of great significance and urgency to develop sensitive and selective sensors for the detection of trace PFOS in water. In this study, a tetraphenylethylene-derived macrocycle BowtieCyclophane has been developed as a fluorescent sensor based on aggregation-induced emission enhancement and fluorochromism. Sensitive detection of PFOS has been achieved with a limit of detection (LOD) of 47.3 ± 2.0 nmol/L (25.4 ± 1.1 µg/L) accompanied by visual fluorescence color changes.
Skeletonema costatum is a diatom widely distributed in red tide microalgae blooms and as one of the main algae causing harmful algal blooms, because of their rapid reproduction and production of toxic and harmful substances, often play a negative role in aquatic ecosystems, and human health and wellbeing. Bacillomycin D is a nonribosomal cyclic antifungal lipopeptide in the iturins family. In this study, Bacillomycin D was tested for its ability to inhibit the growth of S. costatum. The EC50 24h of Bacillomycin D on S. costatum was 24.70 μg/mL. The chlorophyll fluorescence parameters Fv/Fm, Fv/Fo, and yield of the diatoms decreased significantly with increasing concentrations of Bacillomycin D. Study of the mechanism showed that Bacillomycin D induced cell death by changing cell membrane permeability, promoting the release of cellular contents. In this study, transcriptomic analysis showed Bacillomycin D significantly inhibited the photosynthesis and metabolism of S. costatum. These findings investigated the inhibitory effect of Bacillomycin D on the growth of S. costatum and provided a theoretical foundation for the development of new environmentally friendly biological algicide.
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