Latest ArticlesA series of spirooxindole-ferrocene hybrids bearing five or four contiguous chiral centers were designed and synthesized via organocatalysis. In vitro protein binding and cellular proliferation assays suggested that compound 5d was the most potent mouse double minute 2 homolog (MDM2) inhibitor. In addition, mechanistic studies indicated that compound 5d suppressed MDM2-mediated p53 degradation, induced apoptosis and promoted oxidative damage. Molecular docking studies have suggested that 5d binds to MDM2 by mimicking the Trp23 and Leu26 residues of p53. This work can provide a basis for the development of novel multifunctional MDM2 inhibitors. The further exploration of more derivatives from this library and additional investigation of organocatalysis application in the development of new molecules may generate new potential lead compounds for cancer-targeted therapy.
Photoelectrochemical (PEC) technology is considered to be a promising approach for solar-driven hydrogen production with zero emissions. Bismuth vanadate (BiVO4) is a kind of photocatalytic material with strong photoactivity in the visible light region and appropriate band gap for PEC water splitting. However, the solar-to-hydrogen efficiency (STH) of BiVO4 is far away from the 10% target needed for practical application due to its poor charge separation ability. Therefore, this review attempts to summarize the strategies for improving the photocurrent density and especially hydrogen production of BiVO4 materials through PEC techniques in the last three years, such as doping nonmetal and metal elements, depositing noble metals, constructing heterojunctions, coupling with carbon and metal-organic framework (MOF) materials to further enhance the PEC performance of BiVO4 photoanode. This review aims to serve as a general guideline to fabricate highly efficient BiVO4-based materials for PEC water splitting.
Transition-metal oxides are considered to be a promising anode material for lithium-ion batteries (LIBs) due to their high capacities, low cost, and ease of synthesis. Herein, a hybrid nanosheet composed of uniform MoO2 nanoparticles (NPs) homogeneously immobilized on the reduced graphene oxide nanosheets (MoO2 NP@rGO) is first synthesized by a self-templating and subsequent calcination treatment. The unique two-dimensional hybridnanosheets provides several merits. rGO can be used as a favorable support for the loading of electrochemically active MoO2 NPs. Meanwhile, MoO2 NPs can effectively prevent the stacking of the rGO. The effective combination of MoO2 NPs and rGO nanosheets furnish additional electrochemically interfacial active sites for extra lithium ion storage. Noticeably, the as-fabricated hybrid nanosheets deliver a reversible capacity of 641 mAh/g after 350 cycles at a current density of 1000 mA/g with a good rate capability. The greatly enhanced lithium storage properties of MoO2 NP@rGO indicate the importance of elaborate construction of novel hybrid hierarchical structures.
To better understand the spatial distribution of brain functions, we need to monitor and analyze neuronal activities. Electrophysiological technique has provided an important method for the exploration of some neural circuits. However, this method cannot simultaneously detect the activities of nerve cell groups. Therefore, methods that can monitor the spatial distribution of neuronal population activity are demanded to explore brain functions. Voltage-sensitive dyes (VSDs) shift their absorption or emission optical signals in response to different membrane potentials, allowing assessing the global electrical state of neurons. Optical recording technique coupled with VSDs is a promising method to monitor the brain functions by detecting optical signal changes. This review focuses on the fast and slow responses of VSDs to membrane potential changes and optical recordings utilized in the central nervous system. In this review, we attempt to show how VSDs and optical recordings can be used to obtain brain functional monitoring at high spatial and temporal resolution. Understanding of brain functions will not only greatly improve the cognition of information transmission of complex neural network, but also provide new methods of treating brain diseases such as Parkinson's and Alzheimer's diseases.
An enzyme-responsive polysaccharide supramolecular targeted nanoassembly was successfully constructed by the host-guest complexation of positively charged mono-(6-(tetraethylenepentamine)-6-deoxy)-β-cyclodextrin (TEPA-CD) with adamantane-grafted hyaluronic acid (HA-ADA). Possessing a series of positively charged polyamine chains, the obtained polysaccharide nanoassembly could serve as a biocompatible plasmid DNA (pDNA) container. More interestingly, the pDNA could be released from the nanoassembly through the enzymatic degradation of HA skeleton, which realized the controlled pDNA binding and release. Besides, the polysaccharide nanoassembly exhibited lower cytotoxicity than the commercial transfection reagents 25kDa bPEI (PEI25k), accompanied by similar gene delivery effect. We believe that this work might present a convenient method for targeted, controlled gene delivery.
Hydrogen-atom-transfer (HAT) is an efficient way for direct C—H functionalization of inert C—H bonds, therefore it has attracted great interests in recent years. So far, various HAT catalysts have been developed. Among them, quinuclidine and its derivatives show different characters toward other HAT catalysts as they tend to abstract electron-rich and hydridic hydrogens in the presence of weak and neutral C—H bonds. These features enable direct C—H functionalization of compounds with various groups which are unable or difficult by other methods. This review summarizes recent advance of photoinduced reactions with quinuclidine and its derivatives as HAT catalysts and exhibits powerful synthetic potential by using quinuclidine and its derivatives as HAT catalysts.
Energy transfer and electron transfer are both fundamental mechanisms enabling numerous functional materials and applications. While most materials systems employ either energy transfer or electron transfer, the combined effect of energy and electron transfer processes in a single donor/acceptor system remains largely unexplored. Herein, we demonstrated the energy transfer followed by electron transfer (ETET) process in a molecular dyad TPE-NBD. Due to energy transfer, the fluorescence of TPE-NBD was greatly enhanced in non-polar solvents. In contrast, polar solvents activated subsequent electron transfer and markedly quenched the emission of TPE-NBD. Consequently, ETET endows TPE-NBD with significant polarity sensitivities. We expect that employing ETET could generate many functional materials with unprecedented properties, i.e., for single laser powered multicolor fluorescence imaging and sensing.
We have developed a MUC1 antigen-based antitumor vaccine loaded on alum colloid encapsulated inside β-glucan particles (GP-Al). The constructed vaccine induced strong MUC1 antigen specific IgG antibody titers and enhanced CD8+ T cells cytotoxic effect to kill tumor cells. These results indicated that GP-Al can be served as an efficient delivery system and adjuvant for the development of cancer vaccines especially small molecule antigens based cancer vaccines.
Cyclin-dependent kinases 4 and 6 inhibitors (CDK4/6i) have been demonstrated to trigger antitumor immunity for tumor regression. However, the therapeutic performance of CDK4/6i-meadiated cancer immunotherapy was impaired by the immunosuppressive tumor microenvironment (ITM) due to overexpression of programmed death ligand 1 (PD-L1) on the surface of cancer cell membrane. To improve the immunotherapeutic performance of CDK4/6i, we herein developed endosomal acid-activatable micelleplex for siRNA delivery and PD-L1 knockdown in the tumor cells in vitro and in vivo. We further demonstrated that the combination of PD-L1 knockdown and CDK4/6 inhibition facilitated intratumoral infiltration of cytotoxic T lymphocytes (CTLs), and elicited protective immune response and efficiently suppressed tumor growth in vivo. This study revealed the importance of molecular design of the micelleplex for highly efficient siRNA delivery, which might provide a novel insight for RNAi-based cancer immunotherapy.
Two-dimensional covalent organic framework (COF) has distinctive properties that offer potential opportunities for developing advanced electrode materials. In this work, a core-shell material composed of TAPB-DMTP-COF (TAPB, 1, 3, 5-tris(4-aminophenyl)benzene; DMTP, 2, 5-dimethoxyterephaldehyde) core and conducting polymer shell, TAPB-DMTP-COF@PANI, was synthesized solvothermally using a polymerization method. The structural characteristics of the prepared composite were revealed by X-ray diffraction patterns (XRD), fourier transform infrared spectra (FTIR), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM). The electrochemical analyses were verified by subsequent monitoring of trace levels of acetaminophen. This resultant composite not only facilitated acetaminophen to interact with absorption sites by π-π stacking effect and hydrogen bonding but also overcame the poor conductivity of COF. Under the optimal conditions, a low limit of detection of 0.032 μmol/L and wide linear range of 0.10-500 μmol/L were obtained. The electrochemical platform was almost unaffected by other interfering substances, and successfully applied for the practical detection of acetaminophen in commercial tablet, human blood serum and urine. The enhanced performance makes this COF based core-shell composite a promising material in electrochemical sensor.
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