Latest ArticlesA visible-light-induced chemoselective reactions of quinoxalin-2(1H)-ones with alkylboronic acids in the presence of air (O2) and N2 atmosphere was developed under transition-metal free conditions, providing 3-alkylquinoxalin-2(1H)-ones and 3, 4-dihydroquinoxalin-2(1H)-ones, respectively. The overall strategy accommodates a broad scope of substituted quinoxalin-2(1H)-ones and alkylboronic acids with good to excellent product yields.
Nickel/(S)-t-Bu-PHOX complex catalyzed asymmetric arylative cyclization of N-alkynones has been achieved, delivering 1, 2, 3, 6-tetrahydropyridines containing a chiral tertiary alcohol in high yields and excellent enantioselectivities, which provides efficient access to chiral tetrahydropyridine and piperidine analogues.
The development of robust photocatalytic systems is key to harvest the solar power for hydrogen production. In the current study, a series of aluminum-based porphyrinic metal organic frameworks (Al-TCPP) with various morphologies of bulk, carambola-like and nanosheets are synthesized with modulated layer thickness. Morphology-dependent photocatalytic activities in hydrogen production are witnessed and inversely correlate to the thickness of the Al-TCPP micro-platelets or nanosheets. Particularly, the exfoliated metal organic layers (MOLs) of Al-TCPP demonstrated a high hydrogen yield rate of 1.32 × 104 µmol h−1 g−1 that is 21-fold of that from the bulk catalyst, as well as an exceptional TON of 6704 that seldom seen in literature. Through comprehensive photochemical characterizations, the remarkable photocatalytic performance of Al-TCPP-MOL is attributed to the great charge separation efficiency and transfer kinetics endowed by the ultrathin 2D morphology with extended active surface area.
Glutathione (GSH) plays a critical role in maintaining cellular redox homeostasis in biological system. Mitochondrion is a pivotal organelle for cellular aerobic respiration and its disorder is associated with impaired redox balance, leading to cell death. In this work, we designed and synthesized a non-invasive "off-on" mitochondrial-targeting fluorescent probe QZ for the detection of GSH in living cells. Based on the mechanism of native chemical ligation (NCL) and fluorescence resonance energy transfer (FRET), a rhodamine B derivative, QZ was prepared, by choosing aromatic thioester bond as the selective reaction site. QZ exhibited excellent detection capability for GSH over Cys and Hcy. Upon addition of GSH to QZ solution, a remarkably enhanced fluorescence was observed with a limit of detection of 2.98 μmol/L. Furthermore, QZ was found to possess the specific mitochondrial localization ability in cell imaging experiments. Moreover, with exogenous and endogenous stimulations, QZ could image GSH in living cells.
Surface deposition based on metal-phenolic networks (MPNs) has received increasing interest in recent years. The catechol structure is generally considered to be essential to the formation of MPNs. Our most recent results have demonstrated that some kinds of monophenols can form MPNs on substrate surfaces. Herein, we report a fast and effective surface-coating system based on the coordination of 3-(4-hydroxy-3-methoxyphenyl)-2-propenoic acid, a kind of monophenol, with Fe3+. Compared with other metal ions such as Cu2+ and Ni2+, Fe3+ with stronger electron acceptability can coordinate with the monophenol more strongly to form MPNs, and moreover, the deposition time significantly decreases to 40 min from generally 24 h. It is demonstrated that the deposition process is controlled by the coordination, Fe3+ hydrolysis, and deprotonation of the monophenol. The coatings endow substrates such as polypropylene microfiltration membrane with underwater superoleophobicity, which can be applied in oil/water separation with high separation efficiency and great long-term stability. In addition, the coated membranes are positively charged and thus are useful in selective adsorption of dyes. The present work not only provides a novel, fast, and one-step deposition method to fabricate MPNs, but also demonstrates that the fabrication efficiency of monophenol-based MPNs is comparable with that of polyphenol-based MPNs.
Drug delivery systems (DDS) are used to deliver therapeutic drugs to improve selectivity and reduce side effects. With the development of nanotechnology, many nanocarriers have been developed and applied to drug delivery, including mesoporous silica. Mesoporous silica nanoparticles (MSNs) have attracted a lot of attention for simple synthesis, biocompatibility, high surface area and pore volume. Based on the pore system and surface modification, gated mesoporous silica nanoparticles can be designed to realize on-command drug release, which provides a new approach for selective delivery of antitumor drugs. Herein, this review mainly focuses on the "gate keepers" of mesoporous silica for drug controlled release in nearly few years (2017–2020). We summarize the mechanism of drug controlled release in gated MSNs and different gated materials: inorganic gated materials, organic gated materials, self-gated drug molecules, and biological membranes. The facing challenges and future prospects of gated MSNs are discussed rationally in the end.
As a worldwide public health issue, chronic kidney disease still lacks of effective therapeutic approaches due to the challenges in conventional organ transplantation and dialysis. Renal tissue engineering offers an advantageous therapeutic or regenerative option over typical donor organ. However, despite the great progress of decellularized extracellular matrix based scaffold for the renal regeneration, several safety concerns and complex composition still remain to be addressed. Herein, the extracellular matrix-mimicking hydrogel scaffolds were developed through covalent and physical cross-linking between swim bladder-derived natural collagen (COL) and anti-fibrosis chondroitin sulfate (CS) derivatives. The biomimetic hydrogels showed proper mechanical property, excellent thermal stability and high biocompatibility both in vitro and in vivo, by altering the mass ratio of COL and CS. When implanted in partially nephrectomized rat model, the 1COL/2CS scaffold enable it recruit more native kidney cells, reduce the tubular damage, and even induce the regeneration of renal tubular-like tissue and restore renal metabolic function more effectively comparing with the pure 2COL and 2CS scaffold. These results suggest that the biomimetic scaffold is a promising functional platform for treating renal diseases.
The effective detecting ONOO− variations in vivo is of great importance to well understand the complex pathophysiological processes. We reported here a photoacoustic (PA) probe AZB-1 for imaging ONOO− in vivo. AZB-1 showed an originally strong photoacoustic signal at 660 nm. And its PA signal can be turned off by shutting the ICT effect caused by the conjugated electron withdrawing group at 2-position of the aza-BODIPY core. Moreover, the probe was successfully employed to imaging ONOO− variations in inflammatory mice models. Wisely utilized this strategy may serve as powerful platforms for the preparation of novel PA chemosensors.
Photophysical properties of organic and organometallic luminophors are closely related with their molecular packings, enabling the exploitation of stimuli-responsive functional luminescent molecules. Mechanochromic molecules, which can change their luminescence characteristics after mechanical stimulus, have received an increasing interest due to their promising applications in multifunctional sensors and molecular switches. During the past two decades, the development of gold(I) chemistry has been attracting the attention of plenty of researchers. Indeed, a variety of gold(I) complexes with fascinating photophysical behaviors have been discovered. This review focuses on the research progress in the different types of mechanoluminochromic gold(I) complexes, including mono-, bi- and multi-nuclear gold(I) systems. Their interesting luminescence behaviors of these gold(I)-containing luminogens upon mechanical stimulus and the proposed mechanisms of their observed mechanochromic luminescence are summarized systematacially. Moreover, this review will put forward an outlook about the possible opportunities and challenges in this significative scientific field.
More and more attentions have been attracted by lithium-sulfur batteries (Li-S), owing to the high energy density for the increasingly advanced energy storage system. While the poor cycling stability, due to the inherent polysulfide shuttle, seriously hampered their practical application. Recently, some polar hosts, like single metal oxides and sulfides, have been employed as hosts to interact with polysulfide intermediates. However, due to the inherent poor electrical conductivity of these polar hosts, a relatively low specific capacity is obtained. Herein, a spinel-type bimetal sulfide NiCo2S4 through a Prussian blue analogue derived methodology is reported as the novel host of polysulfide, which enables high-performance sulfur cathode with high Coulombic efficiency and low capacity decay. Notably, the Li-S battery with NiCo2S4-S composites cathode still maintains a capacity of 667 mAh/g at 0.5 C after 300 cycles, and 399 mAh/g at 1 C after 300 cycles. Even after 300 cycles at the current density of 0.5 C, the capacity decays by 0.138% per cycle at high sulfur loading about 3 mg/cm2. And the capacity decays by 0.026% per cycle after 1000 cycles, when the rate is 1 C. More importantly, the cathode of NiCo2S4-S composite shows the outstanding discharge capacity, owing to its good conduction, high catalytic ability and the strong confinement of polysulfides.
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