Latest ArticlesHeterogeneous transition metal catalysts are indispensable in improving environmental pollution. However, their fabrication is often costly and cumbersome, and they can easily pollute the environment. This study proposed using a natural Gabonese ore (GBO) containing MnxOy and FexOy as catalysts to degrade orange Ⅱ (OII) via peroxymonosulfate (PMS) activation. The GBO + PMS system exhibited extraordinarily high stability and catalytic activity towards OII elimination (92.2%, 0.0453 min−1). The reactive oxygen species (ROS) generated in the system were identified using radical scavenging tests and electron spin-resonance (ESR) analysis. Singlet oxygen (1O2) represented the dominant reactive species for OII degradation, while the system presented a lower reaction energy barrier and was effective in a broad pH range (2–10). This work also proposed the activation mechanism for the GBO + PMS system and OII degradation pathways. This study revealed a new approach for exploring inexpensive, eco-friendly, efficient, and stable heterogeneous transition metal catalysts.
An efficient and catalytic protocol for highly stereoselective construction of β-mannopyranosylation has been developed. Glycosylation of 2,6-lactone-bridged mannopyranosyl ortho-hexynylbenzoate with various acceptors proceeded smoothly in the presence of 5% Hg(Ⅱ) at room temperature, resulting in the corresponding β-mannosides in high yield and exclusive β-stereoselectivity.
A novel type of host–guest recognition systems have been developed on the basis of a Au(Ⅲ) molecular tweezer receptor and chiral Pt(Ⅱ) guests. The complementary host–guest motifs display high non-covalent binding affinity (Ka: ~104 L/mol) due to the participation of two-fold intermolecular π–π stacking interactions. Both phosphorescence and chirality signals of the Pt(Ⅱ) guests strengthen in the resulting host–guest complexes, because of the cooperative rigidifying and shielding effects rendered by the tweezer receptor. Their intensities can be reversibly switched toward pH changes, by taking advantage of the electronic repulsion effect between the protonated form of tweezer receptor and the positive-charged guests in acidic environments. Overall, the current study demonstrates the feasibility to enhance and modulate phosphorescence and chirality signals simultaneously via molecular tweezer-based host–guest recognition.
In recent years, the direct introduction of sulfonyl and sulfenyl groups into unsaturated substrates by using thiosulfonates as unique dual functional reagents has inarguably provided chemists a new platform for the diverse synthesis of important S-containing derivatives. These 1,n-thiosulfonylation reactions usually feature simple procedures, 100% atom economy, and high regioselectivity. This review focuses on the recent advancements in the transformations of thiosulfonates through 1,n-thiosulfonylation involving the formation of two distinct C-S bonds under transition-metal-catalyzed or metal-free conditions, where thiosulfonates act as both a sulfonyl and a sulfenyl component.
Inflammatory bowel disease (IBD) is a chronic and recurrent disease of the gastrointestinal tract, mainly including Crohn's disease (CD) and ulcerative colitis (UC). However, current approaches against IBD do not precisely deliver drugs to the inflammatory site, which leads to life-long medication and serious side effects that can adversely impact patients' adherence. It is necessary to construct optimal drug delivery systems (DDSs) that can target drugs to the region of inflammation, thereby improve therapeutic efficacy and reduce side effects. With the burgeoning development of nanotechnology-based nanomedicines (NMs) and prodrug strategy, remarkable progresses in the treatment of IBD have been made in recent years. Herein, the latest advances are outlined at the intersection of IBD treatment and nanotherapeutics as well as prodrug therapy. First, the pathophysiological microenvironment of inflammatory sites of IBD is introduced in order to rationally design potential NMs and prodrugs. Second, the necessity of NMs for the IBD therapy is elaborated, and the representative nanotherapeutics via passive targeted and active targeted NMs developed to treat the IBD are overviewed. Furthermore, the emerging prodrug-based therapeutics are summarized, including 5-aminosalicylic acid-, amino acid-, and carbohydrate-conjugated prodrugs. Finally, the design considerations and perspectives of these NMs and prodrugs-driven IBD therapeutics in the clinical translation are spotlighted.
Drug-induced liver injury (DILI) is a common and serious adverse drug reaction. At present, DILI is perfectly diagnozed in clinical settings using Roussel Uclaf causality assessment method (RUCAM) in its original version published 1993 and its updated version published 2016, well established worldwide as a diagnostic algorithm with a high sensitivity and specificity. Nevertheless, the search for additional detection methods supporting RUCAM continues. In recent years, with the development of optical imaging technology, fluorescent probes have gradually shown great advantages in the detection and diagnosis of DILI markers such as high sensitivity, anti-interference, real-time monitoring and non-invasive measurement. In this review, the recent advances of fluorescent probes for evaluation of DILI in experimental studies were summarized according to various markers of DILI. We believe that learning about the design and practical application of these probes will contribute to the further development of detection sensors for DILI markers.
Peroxide ligation of aqueous metal–oxo clusters provides rich speciation and structural diversity. Here, three novel transition-metal derivatives of polyoxometalate anions, [Ni2(H2O)10{P4Ta6(O2)6O24}]6– (1a), [Zn(H2O)4{P4Ta6(O2)6O24}]8– (2a) and [Cd(H2O)4{P4Ta6(O2)6O24}]8– (3a), have been successfully synthesized by adopting a one-pot reaction strategy. All of these hexatantalates are built from a new-type phosphorus-incorporated hexatantalates. We investigated the solution behaviors, and the peak assignments of the MS spectra indicated some degree of stability of them in water. Furthermore, the proton-conducting ability of compound 1a was also explored and it has shown well conductivity at high relative humidities, with conductivity achieved 1.22 × 103 S/cm (85 ℃, 90%RH).
The applications of fluorescence resonance energy transfer (FRET) are coming to be one of the simplest and most accessible strategy with super-resolved optical measurements. Meanwhile, nanomaterials have become ideal for constructing FRET-based system, due to their unique advantages of tunable emission, broad absorption, and long fluorescence (FL) lifetime. The limitations of traditional FRET-based detections, such as the intrinsic FL, auto-FL, as well as the short FL lifetime, could be overcome with nanomaterials. Consequently, numbers of FRET-based nanomaterials have been constructed for precise, sensitive and selective detections in biological systems. They could act as both energy donors and/or acceptors in the optical energy transfer process for biological detections. Some other nanomaterials would not participate in the energy transfer process, but act as the excellent matrix for modifications. The review will be roughly classified into nanomaterial-involved and uninvolved ones. Different detection targets, such as nucleic acids, pathogenic microorganisms, proteins, heavy metal ions, and other applications will be reviewed. Finally, the other biological applications, including environmental evaluation and mechanism studies would also be summarized.
Electrochemical nitrogen reduction reaction (NRR) has been considered as an appealing and sustainable method to produce ammonia from N2 under ambient conditions, attracting increasing interest. Limited by low solubility of N2 in water and high stability of NN triple bond, developing NRR electrocatalysts with both strong N2 adsorption/activation and high electrical conductivity remain challenging. Here, we demonstrate an efficient strategy to develop NRR electrocatalyst with synergistically enhanced N2 adsorption/activation and electrical conductivity by heteroatom doping. Combining computational and experimental study, the DFT-designed Ti-doped SnO2 exhibits significantly enhanced NRR performance with ammonia yield rate of 13.09 µg h−1 mg−1 at −0.2 V vs. RHE. Particularly, the Faradaic efficiency reaches up to 42.6%, outperforming most of Sn-based electrocatalysts. The fundamental mechanism for improving NRR performance of SnO2 by Ti doping is also revealed. Our work highlights a powerful strategy for developing high-activity electrocatalysts for NRR and beyond.
Electrochemical reduction of CO2 to value-added chemicals holds promise for carbon utilization and renewable electricity storage. However, selective CO2 reduction to multi-carbon fuels remains a significant challenge. Here, we report that B/N-doped sp3/sp2 hybridized nanocarbon (BNHC), consisting of ultra-small nanoparticles with a sp3 carbon core covered by a sp2 carbon shell, is an efficient electrocatalyst for electrochemical reduction of CO2 to ethanol at relatively low overpotentials. CO2 reduction occurs with a Faradaic efficiency of 58.8%-69.1% for ethanol and acetate production at -0.5 ~ -0.6 V (vs. RHE), among which 51.6%-56.0% is for ethanol. The high selectivity for ethanol is due to the integrated effect of sp3/sp2 carbon and B/N doping. Both sp3 carbon and B/N doping contribute to enhanced ethanol production with sp2 carbon reducing the overpotential for CO2 reduction to ethanol.
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