Latest ArticlesThirteen new fluorine-containing drugs, which have been granted approval by the US Food and Drug Administration (FDA) in 2020, are profiled in this review. Therapeutic areas of these new fluorinated pharmaceuticals include medicines and diagnostic agents for Cushing's disease, neurofibromatosis, migraine, Alzheimer's disease, myelodysplastic syndromes, hereditary angioedema attacks, and various cancers. Molecules of these approved drugs feature aromatic fluorine (Ar-F) (11 compounds), aromatic Ar-CF3 (1), aliphatic CHF (1) and CF2 (1) groups. For each compound, we provide a spectrum of biological activity, medicinal chemistry discovery, and synthetic approaches.
Dopamine (DA) is easy to be oxidized and polymerizes to form polydopamine (pDA) in alkaline conditions, while the synthesis is usually time-consuming (48 h). Herein, the polymerization of DA is completed with 4 h under the catalysis of acid phosphatase (ACP). The high efficiency makes the detection of DA feasibility based on the self-polymerization of DA. In this assay, pDA is grown in situ on the surface of covalent organic frameworks (COFs), and then the fluorescence of COFs is quenched significantly. The linear range of DA is achieved from 0.5–50 μmol/L with a detection limit of 0.16 μmol/L. The detection of DA is not interfered with uric acid, ascorbic acid, and some phenolic compounds, because these substances cannot polymerize in the presence of ACP. Moreover, benefiting from the good sensitivity and selectivity, DA has been successfully determined by this strategy in human urine samples with satisfactory recoveries.
The conversion of CO2 under mild condition is of great importance because these reactions involving CO2 can not only produce value-added chemicals from abundant and inexpensive CO2 feedstock but also close the carbon cycle. However, the chemical inertness of CO2 requires the development of high-performance catalysts. Herein, Ag nanoparticles/MIL-100(Fe) composites were synthesized by simple impregnation-reduction method and employed as catalysts for the photothermal carboxylation of terminal alkynes with CO2. MIL-100(Fe) could stabilize Ag nanoparticles and prevent them from aggregation during catalytic process. Taking the advantages of photothermal effects and catalytic activities of both Ag nanoparticles and MIL-100(Fe), various aromatic alkynes could be converted to corresponding carboxylic acid products (86%–92% yields) with 1 atm CO2 at room temperature under visible light irradiation when using Ag nanoparticles/MIL-100(Fe) as photothermal catalysts. The catalysts also showed good recyclability with almost no loss of catalytic activity for three consecutive runs. More importantly, the catalytic performance of Ag nanoparticles/MIL-100(Fe) under visible light irradiation at room temperature was comparable to that upon heating, showing that the light source could replace conventional heating method to drive the reaction. This work provided a promising strategy of utilizing solar energy for achieving efficient CO2 conversion to value-added chemicals under mild condition.
Heterogeneous nanostructures that are defined as a hybrid structure consisting of two or more nanoscale domains with distinct chemical compositions or physical characteristics have attracted intense efforts in recent years. In this review, we focus on the introduction of a number of heterogeneous nanostructures derived using core-shell Ag-Pt nanoparticles as starting materials, including hollow, dimeric and composite structures and also highlight their application in catalyzing electrochemical reactions, e.g., methanol oxidation reaction and oxygen reduction reaction. This review not only shows the capability of core-shell Ag-Pt nanoparticles in producing various heterogeneous nanostructures as starting templates, but also highlights the structural design or electronic interaction that endows the heterogeneous nanostructures with enhanced catalytic properties either in methanol oxidation or in oxygen reduction. Further, we also make some perspectives for more heterogeneous nanostructures that may be prepared by using core-shell Ag-Pt particles or their derivatives so as to offer the readers the opportunities and challenges in this field.
Although magnetic stirring is frequently used to enhance the kinetics for adsorption, chemical and biochemical reactions, the introduction of stirrers inevitably leads to the adsorption of analytes and thus interferes with the efficiency of the chemical process or reaction. In this work, magnetic Fe3O4 nanorods with tunable length-to-diameter ratio were synthesized via a hydrothermal method and used as templates for the in-situ depositing of MIL-100(Fe) and gold nanoparticles. Such nanorod-based material can not only function as an adsorbent, nanozyme, and a heterogeneous catalyst for corresponding applications but also serve as a magnetic nanostirrer to enhance kinetics. As a proof-of-concept, the capture of bacteria pathogen, mimic-peroxidase-based colorimetric detection of hydrogen peroxide, and the catalytic reduction of selected organic pollutants were conducted using the as-synthesized Fe3O4@MIL-100(Fe)-Au nanostirrer with and without magnetic field. The results show that the rates of bacteria capture, mimetic enzyme reaction and catalysis were tremendously expedited. We believe this magnetic field-assisted approach holds great promise for future applications, because, not only does it eliminate the use of external magnetic stirrers and thereby decrease the risk of foreign pollution but also, is adaptable for nanoscale reaction systems where conventional stirring is not applicable due to size limitations.
A novel hydrogen-bonded organic frameworks (HOFs) FJU-200 has been constructed from N, N'-bis(5-isophthalic acid)naphthalimide (H4L). FJU-200 has a good dual-function of aniline and ultraviolet detection. FJU-200 is the first case of HOF with dual sensing of visual color changes and photoluminescence quenching for aniline detection, and the detection limit of aniline can reach 5.5 × 10−4 mol/L. Under ultraviolet FJU-200 will rapidly change from light yellow to rustic brown, which makes it possible to use FJU-200 to achieve minute-level ultraviolet detection. Moreover, for more convenient use, FJU-200 test papers are prepared. Using them, convenient and fast aniline or ultraviolet detection can be realized. The single-crystal X-ray structures show that compared with the original FJU-200, both and UV-FJU-200 have larger pore sizes, and the dihedral angles of the H2L2− in framework has been changed.
In this paper, a novel BC3N2 monolayer has been found with a graphene-like structure using the developed particle swarm optimization algorithm in combination with ab initio calculations. The predicted structure meets the thermodynamical, dynamical, and mechanical stability requirements. Interestingly, the BC3N2 plane shows a metallic character. Importantly, BC3N2 has an in-plane stiffness comparable to that of graphene. We have also investigated the adsorption characteristics of CO2 on pristine monolayer and Mo functionalized monolayer using density functional theory. Subsequently, electronic structures of the interacting systems (CO2 molecule and substrates) have been preliminarily explored. The results show that Mo/BC3N2 has a stronger adsorption capacity towards CO2 comparing with the pristine one, which can provide a reference for the further study of the CO2 reduction mechanism on the transition metal-functionalized surface as well as the new catalyst's design.
Numerous researchers have paid attention to achieve metal-free phosphorescence by exploring new structures or new mechanisms. Herein, a facile way is introduced to endow a common fluorescence dye, tetrabromofluorescein (4Br-Flu), some fabulous optical characteristics such as dual emission including thermally activated delayed fluorescence, room-temperature phosphorescence (RTP), and the excellent pH-sensitivity. Shortly, 4Br-Flu with good light-emitting properties is composed into the polymer system. The multiple bromine atoms promote the spin-orbit coupling effect and facilitate triplet excitation. Especially, the hydrogen bonding network of the polymer restricts the molecular motion of 4Br-Flu so that the system can emit long-wavelength RTP when 4Br-Flu is doped into polyvinyl alcohol or co-polymerized with acrylamide. Due to the reversible transformation of protonation and deprotonation, the 4Br-Flu based polymer responded to acid and alkali like a phosphorescent switch which makes it an excellent hydrogen chloride/ammonia gas leak detector in dry environment.
Database-assisted global metabolomics has received growing attention due to its capability for unbiased identification of metabolites in various biological samples. Herein, we established a mass spectrometry (MS)-based database-assisted global metabolomics method and investigated metabolic distance between pleural effusion induced by tuberculosis and malignancy, which are difficult to be distinguished due to their similar clinical symptoms. The present method utilized a liquid chromatography (LC) system coupled with high resolution mass spectrometry (MS) working on full scan and data dependent mode for data acquisition. Unbiased identification of metabolites was performed through mass spectral searching and then confirmed by using authentic standards. As a result, a total of 194 endogenous metabolites were identified and 33 metabolites were found to be differentiated between tuberculous and malignant pleural effusions. These metabolites involved in tryptophan catabolism, bile acid biosynthesis, and β-oxidation of fatty acids, provided non-invasive biomarkers for differentiation of the pleural effusion samples with high sensitivity and specificity.
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