Latest ArticlesPhotoelectrochemical (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.
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.
Vaccine adjuvants have been widely used to enhance the immunogenicity of the antigens and elicit long-lasting immune response. However, only few vaccine adjuvants have been approved by the FDA for human use so far. Therefore, there is still an urgent need to develop novel adjuvants for the potential applications in clinical trials. Herein, non-nucleotide small molecule STING agonist diABZI was employed to construct glycopeptide antigen based vaccines for the first time. Immunological evaluation indicated diABZI not only enhanced the production of antibodies and T cell immune responses, but also inhibited tumor growth in tumor-bearing mice in glycopeptide-based subunit vaccines. These results indicated that di-ABZI demonstrates a high potential as adjuvant for the development of cancer vaccines.
Amphichoterpenoids A–C (1–3), unprecedented picoline-derived meroterpenoids possessing a pyrano[3, 2-c]pyridinyl-γ-pyranone scaffold, were characterized from the ascidian-derived fungus Amphichorda felina SYSU-MS7908. Their structures were elucidated by spectroscopic methods, X-ray diffraction and electronic circular dichroism (ECD) calculations. A plausible biosynthetic pathway was proposed. The isolated compounds displayed moderate inhibitory activity against acetylcholinesterase with 50% inhibiting concentration (IC50) values of 18.8–53.2 μmol/L.
A 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.
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.
An efficient and eco-friendly protocol for synthesizing difluoromethylated oxindoles through a visible-light induced one-pot tandem reaction of N-arylacrylamides, difluoroacetic acid and PhI(OAc)2 was developed. This reaction proceeded in the absence of any additive, base, metal-catalyst and external photosensitizer, using cheap and easily available CHF2CO2H as the difluoromethylation reagent and bulk biomass-derived 2-MeTHF as the sole solvent. 26 Examples of N-arylacrylamide substrates were investigated, and all of them successfully underwent difluoromethylation to deliver the target products in good to excellent yields.
The reaction of a metallo-organic ligand (LA) in which two "V"-shaped bisterpyridines attaching to meta-position of "X"-shaped tetraterpyridine via < tpy-Ru2+-tpy > connectivity and Zn2+ ions gave rise to 3D supramolecular architectures: octagram (Zn8LA4). However, a position varied ligand (LB) in which two "V"-shaped bisterpyridines locating at the ortho-position of "X"-shaped tetraterpyridine afforded a different 3D hexagram (Zn6LB3). Full characterizations included NMR (1H, 13C, 2D COSY, NOESY and DOSY), ESI-MS, TWIM-MS, TEM and AFM. The resulted structures were directly determined by the position of two "V"-shaped bisterpyridines attaching to "X"-shaped tetraterpyridine.
Novel and efficient Mn(OAc)3·2H2O promoted radical addition-[4+1] cyclization relay of 3-indolymethanols and phosphites was disclosed, which afforded 1, 2-oxaphospholoindole derivatives in moderate to good yields. Based on the experimental and computational studies, a mechanism involving radical addition and intramolecular cyclization cascade was proposed.
4-Hydroxyphenylpyruvate dioxygenase (HPPD) is an important target for both drug and pesticide discovery. As a typical Fe(Ⅱ)-dependent dioxygenase, HPPD catalyzes the complicated transformation of 4-hydroxyphenylpyruvic acid (HPPA) to homogentisic acid (HGA). The binding mode of HPPA in the catalytic pocket of HPPD is a focus of research interests. Recently, we reported the crystal structure of Arabidopsis thaliana HPPD (AtHPPD) complexed with HPPA and a cobalt ion, which was supposed to mimic the pre-reactive structure of AtHPPD-HPPA-Fe(Ⅱ). Unexpectedly, the present study shows that the restored AtHPPD-HPPA-Fe(Ⅱ) complex is still nonreactive toward the bound dioxygen. QM/MM and QM calculations reveal that the HPPA resists the electrophilic attacking of the bound dioxygen by the trim of its phenyl ring, and the residue Phe381 plays a key role in orienting the phenyl ring. Kinetic study on the F381A mutant reveals that the HPPD-HPPA complex observed in the crystal structure should be an intermediate of the substrate transportation instead of the pre-reactive complex. More importantly, the binding mode of the HPPA in this complex is shared with several well-known HPPD inhibitors, suggesting that these inhibitors resist the association of dioxygen (and exert their inhibitory roles) in the same way as the HPPA. The present study provides insights into the inhibition mechanism of HPPD inhibitors.
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