Latest ArticlesThree novel series of α-aminoamides derivatives were designed and synthesized based on ralfinamide, and their Nav1.7 inhibitory activities were evaluated using manual patch clamp electrophysiology. Active compounds inhibited Nav1.7 with half maximal inhibitory concentration (IC50) values ranging from 2.9 µmol/L to 21.4 µmol/L. Among them, the most potent compound 19h exhibited about 12-fold potency better than ralfinamide. The investigation of their structure-activity relationship gives a strategy to improve the Nav1.7 inhibition of ralfinamide analogues. Compound 19h was efficacious in antinociception in the mouse spared nerve injury (SNI) model of neuropathic pain without causing sedation in the open field test.
Benzoyl peroxide (BPO) has been added in wheat flour because of its bleaching effect. However, the abnormal used BPO has caused increasing concern due to its strong oxidization capability which may have adverse effects on living organisms. Herein, we present a carbon dot (CD)-based fluorescent and colorimetric probe for visually, sensitively and selectively sensing BPO. The addition of BPO could quench the red fluorescence of CDs peaked at 622 and 677 nm, and decrease the absorbance at 613 nm, while increase the absorbance at 450 nm, resulting in a fluorescence turn-off and colorimetric spectral response. Moreover, the CDs had short response time of 10 min and high sensitivity towards BPO with a low limit of detection of 28 nmol/L. The applicability of the CDs in detecting BPO in wheat, noodle and starch samples was further demonstrated, and good recovery results were obtained.
Imaging dynamics of membrane proteins of live cells in a wash-free and real-time manner has been a challenging task. Herein, we report unprecedented applications of malachite green (MG), an organic dye widely used in pigment industry, as a switchable fluorophore to monitor membrane enzymes or non-catalytic proteins in live cells. Conformationally flexible MG is non-fluorescent in aqueous solution, yet covalent binding with endogenous proteins of cells significantly enhances its fluorescence at 670 nm by restricting flexibility of dye. Integrating a phosphate-caged quinone methide precursor with MG yielded a covalent labeling fluorogenic probe, allowing real-time imaging of membrane alkaline phosphatase (ALP, a model catalytic protein) activity in live cells with over 100-fold enhancement of fluorescence intensity. Moreover, MG is also applicable to image non-catalytic protein by conjugation with protein-specific ligand. A fluorogenic probe consisted of c-RGDfK peptide and MG proved to be compatible with wash-free and real-time visualization of non-catalytic integrin αvβ3 in live cells with high contrast.
Treatment of bone defects still poses a great challenge in orthopedic clinics, and the vital role of periosteum in such processes has attracted widespread attention. However, studies focusing on the oxidative stress micro-environment with an artificial periosteum at the site of defect have been scarce. The intrinsic anti-oxidative properties and therapeutic potential for bone defects of metal-phenolic networks (MPNs) have provided a potential solution to this. Herein, we have developed a protocatechualdehyde + zinc ion (PCA+ZnⅡ) MPN coating on a thermoplastic polyurethane membrane with a one-pot method to fabricate a new-type of periosteum with meritorious biocompatibility and abilities of modulating oxidative stress condition and promoting osteogenesis and mineralization for better bone regeneration, which has shown to be a promising strategy for constructing artificial periosteum with various MPNs.
Membrane tension plays a significant role in many cellular processes including cell adhesion, migration and spreading. Despite the importance of membrane tension, it remains difficult to measure in vivo. Recently, the development of non-invasive fluorescent probes have made great progress, especially excited-state deplanarization in molecular rotors has been applied to image membrane tension in living cells. Nevertheless, an intrinsic limitation of such kind of probe is that they depend on the lipid packing, and how the lipid packing responds to the membrane tension change remains unclear. Therefore, in this work, we used a polarity-sensitive membrane probe to investigate the possible response mechanism of lipid packing to the change of membrane tension that was regulated by osmotic shocks. The results showed that an increase in membrane tension could stretch the lipids apart with large displacements, and this change was not homogeneous on the whole membrane, instead, increase of membrane tension induced phase separation.
Due to the technology limitation and inferior deNOx efficiency of urea selective catalytic reduction (SCR) catalysts at low temperatures, passive NOx adsorber (PNA) for decrease of NOx, CO and hydrocarbons (HCs) during "cold start" of vehicles was proposed to meet the further tighten NOx emission regulations in future. Among them, Pd modified zeolite PNA materials have received more attention because of their excellent NOx storage capacity, anti-poisoning and hydrothermal stability and since Pd/zeolite PNA was proposed, a variety of advanced characterization methods have been applied to investigate its adsorption behavior and structure-performance relationship. The comprehension of the active sites and adsorption chemistry of Pd/zeolite PNA was also significantly improved. However, there are few reviews that systematically summarize the recent progress and application challenges in atomic-level understanding of this material. In this review, we summarized the latest research progress of Pd/zeolite PNA, including active adsorption sites, adsorption mechanism, material physicochemical properties, preparation methods, storage and release performance and structure-performance relationships. In addition, the deactivation challenges faced by Pd/zeolite PNA in practical applications, such as chemical poisoning, high temperature hydrothermal aging deactivation, etc., were also discussed at the micro-level, and some possible effective countermeasures are given. Besides, some possible improvements and research hotspots were put forward, which could be helpful for designing and constructing more efficient PNA materials for meeting the ultra-low NOx emission regulation in the future.
Nitrogen reduction reaction (NRR) is a clean mode of energy conversion and the development of highly efficient NRR electrocatalysts under ambient conditions for industrial application is still a big challenge. Metal-nitrogen-carbon (M-N-C) has emerged as a class of single atom catalyst due to the unique geometric structure, high catalytic activity, and clear selectivity. Herein, we designed a series of dual metal single atom catalysts containing adjacent M-N-C dual active centers (MN4/M'N4-C) as NRR electrocatalysts to uncover the structure-activity relationship. By evaluating structural stability, catalytic activity, and selectivity using density functional theory (DFT) calculations, 5 catalysts, such as CrN4/M'N4-C (M' = Cr, Mn, Fe, Cu and Zn), were determined to exhibit the best NRR catalytic performance with the limiting potential ranging from −0.64 V to −0.62 V. The CrN4 center acted as the main catalytic site and the adjacent M'N4 center could enhance the NRR catalytic activity by modulation effect based on the analysis of the electronic properties including the charge density difference, partial density of states (PDOS), and Bader charge variation. This study offers useful insights on understanding the structure-activity relationship of dual metal single atom catalysts for electrochemical NRR.
van der Waals (vdWs) heterostructures based on two-dimensional (2D) materials have become a promising candidate for photoelectrochemical (PEC) catalyst not only because of the freedom in materials design that enable the band-offset construction and facilitate the charge separation. They also provide a platform for the study of various of interface effect in PEC. Here, we report a new kind of mixed-dimensional vdWs heterostructure photoelectrode and investigate the strain enhanced PEC performance at vdWs interfaces. Our heterostructures are composed of 2D n-type MoS2 nanosheets and three-dimensional (3D) p-type Cu2O nanorod arrays (NRAs), where Cu2O NRAs introduce periodically strain in the p-n junction interface. We find a promotion of the HER catalytic activities in heterostructure based PEC photoelectrodes using in-situ measurement techniques including the scanning electrochemical cell microscopy and various local spectrum probe measurements. This is attributed to the efficient charge separation at the strained heterointerface. Our results demonstrate an interesting venue for understanding the local interface effects with high spatial resolution, and shed light on design and developing high-efficiency photoelectrodes. 1L MoS2/Cu2O vdWs heterostructure photocathodes were prepared by nanoindentation technology. The effects of strain on promoting charge separation at the heterointerface were verified by the enhanced performances in PEC hydrogen evolution reaction of vdWs heterostructure through scanning electrochemical cell microscopy technique and various local spectrum probe measurements.
Two pairs of Pt(II) enantiomers ((RR)/(SS)-PyPt, ((RR)/(SS)-Py: N, N'-(1, 2-diphenylethane-1, 2-diyl)dipicolinamide; (RR)-P/M-QPt, ((RR)/(SS)-Q: N, N'-((1R, 2R)-1, 2-diphenylethane-1, 2-diyl)bis(quinoline-2-carboxamide)) were synthesized, respectively, with good circularly polarized luminescence (CPL) and tunable dissymmetry factors (g) by molecular self-induction with (RR)/(SS)-1, 2-diphenylethane-1, 2-diamine as carbon chiral sources. In the (RR)-P-QPt and (SS)-M-QPt, specific P- and M-configurations were effectively induced from intrinsic chiral carbon centres (R or S), ingeniously avoiding the racemic mixture formation and chiral separation. Furthermore, the chirality originating from both chiral carbon centres and helicene-like structure improves the g factor significantly, which provides a new molecular design strategy for chiral Pt(II) enantiomers with good CPL properties.
Carbon materials hold the great promise for application in energy storage devices owing to their low cost, high thermal/chemical stability, and high electrical conductivity. However, it remains challenging to synthesize high-performance carbon electrodes in a simple, scalable and sustainable way. Here, we report a facile method for scalable synthesis of porous carbon anode by using cheap and easily accessible zeolitic imidazolate framework-8 as a template and polyvinylpyrrolidone as an additional carbon source. The obtained porous carbon shows the macroscopic sheet-like morphology, which has the highly disordered structure, expanded interlayer spacing, abundant pore structure, and nitrogen doping properties. This porous carbon anode is demonstrated to have the excellent K+ charge storage properties in specific capacity, rate capability, and cycling stability. A potassium-ion capacitor assembled by using this porous carbon as the anode, delivers a maximum energy density of 85.12 Wh/kg and power density of 11860 W/kg as well as long cycle life exceeding 3000 cycles. This represents a critical advance in the design of low cost and scalable carbon material for applications in energy storage devices.
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