Latest ArticlesUnderstanding the dynamic assembly process of DNA nanostructures is important for developing novel strategy to design and construct functional devices. In this work, temperature-controlled dynamic light scattering (DLS) strategy has been applied to study the global assembly process of DNA origami and DNA bricks. Through the temperature dependent size and intensity profiles, the self-assembly process of various DNA nanostructures with different morphologies have been well-studied and the temperature transition ranges could be observed. Taking advantage of the DLS information, rapid preparation of the DNA origami and the brick assembly has been realized through a constant temperature annealing. Our results demonstrate that the DLS-based strategy provides a convenient and robust tool to study the dynamic process of forming hieratical DNA structures, which will benefit understanding the mechanism of self-assembly of DNA nanostructures.
It remains a big challenge to develop solid-state stimuli-responsive materials for time-dependent information encryption and inkless erasable printing with long retention times. Herein, a 2D Cu2I2-based MOF with photoresponsive spiropyran (SP) groups orderly installed on its skeleton is developed. The structural isomerization from SP to colored merocyanine (MC) form can be triggered by removing the CH3CN guests. Besides, the degree of structural isomerization and the retention time can be adjusted by controlling the amount of CH3CN guests, exhibiting dynamic photochromic behavior with multicolor states and tunable retention time. Based on these advantages, time-dependent information encryption is successfully achieved. Furthermore, the long retention time (> 72 h) of the MC form under daylight conditions in the CH3CN-removed Cu2I2-based MOF and good repeatability make it promising in various applications, such as temporary calendars, price-cards, billboards, and reusable identity cards. This work provides a novel design strategy to fabricate multi-functional MOF-based smart materials for challenging applications of time-dependent information encryption and inkless erasable printing.
Thermocatalytic nonoxidative ethane dehydrogenation (EDH) is a promising strategy for ethene production but suffers from intense energy consumption and poor catalyst durability; exploring technology that permits efficient EDH by solar energy remains a giant challenge. Herein, we present that an oxygen vacancy (Ov)-rich LaVO4 (LaVO4-Ov) catalyst is highly active and stable for photocatalytic EDH, through a dynamic lattice oxygen (Olatt.) and Ov co-mediated mechanism. Irradiated by simulated sunlight at mild conditions, LaVO4-Ov effectively dehydrogenates undiluted ethane to produce C2H4 and CO with a conversion of 2.3%. By loading a small amount of Pt cocatalyst, the evolution and selectivity of C2H4 are enhanced to 275 µmol h−1 g−1 and 96.8%. Of note, LaVO4-Ov appears nearly no carbon deposition after the reaction. The isotope tracked reactions reveal that the consumed Olatt. recuperates by exposing the used catalyst with O2, thus establishing a dynamic cycle of Olatt. and achieving a facile catalyst regeneration to preserve its intrinsic activity. The refreshed LaVO4-Ov exhibits superior reusability and delivers a turnover number of about 305. The Ov promotes photo absorption, boosts ethane adsorption/activation, and accelerates charge separation/transfer, thus improving the photocatalytic efficiency. The possible photocatalytic EDH mechanism is proposed, considering the key intermediates predicted by density functional theory (DFT) and monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS).
Oral squamous cell carcinoma (OSCC) is known as one of the most malignant tumors with high recurrence and fatality rate. The poor tumor-targeting ability of traditional chemotherapeutic drugs has been a grand challenge for anti-OSCC therapy. Beyond that, a large quantity of tumor associated macrophages in OSCC tissues further diminish the anti-tumor effects of these drugs. Therefore, we produced a therapeutic nano drug delivery system (FA-PEG-PLA-JQ1) through encapsulating JQ1 [a small-molecule inhibitor of bromodomain containing protein 4 (BRD4)] into the folic acid (FA)-modified nanoparticle (PEG-PLA), which could prolong the half-life of JQ1 and target the tumor tissues. And then, JQ1 released from this nanoparticle could prevent OSCC growth inducing tumor cell apoptosis, inhibiting tumor angiogenesis and the polarization of M2 type macrophages. In conclusion, our date demonstrated the therapeutic benefits of FA-PEG-PLA-JQ1 against OSCC in vivo or in vitro, which could be a novel treatment strategy for OSCC in coming days.
Human Notum (hNotum) inhibitors could be used for treating Wnt signalling-associated diseases including colorectal cancer. Herein, two series of chalcone derivatives were designed and synthesized aiming to find selective and potent hNotum inhibitors. Structure–activity relationship (SAR) studies showed that 2-methoxyl and 5-bromine substitutions on A-ring significantly enhanced anti-hNotum effect, while 4′-ethoxyl and 3′-alkyl substitutions on B-ring were beneficial for hNotum inhibition. Among all tested chalcones, B11 displayed the most potent anti-Notum effect (IC50 = 3.6 nmol/L), good selectivity, excellent chemical stability and suitable metabolic stability. Further investigations showed that B11 acted as a competitive inhibitor of hNotum, while this agent (5 µmol/L) significantly weaken the migration abilities of colorectal cancer cells. Collectively, this study deciphers the SARs of chalcones as hNotum inhibitors and reports a novel and potent hNotum inhibitor with the anti-migration effect on colorectal cancer cells, which offers a promising lead compound to develop novel anti-cancer agents.
Here, we report a concise and divergent enantioselective total synthesis of marine sesquiterpene quinone meroterpenoids (+)-dysidavarones A–C (1–3) using predysidavarone 6 as a key common intermediate. The highly strained and bridged eight-membered carbocycle of predysidavarone 6 was constructed by a one-pot intermolecular alkylation and intramolecular arylation of Wieland–Miescher ketone derivative 11 and benzyl bromide 12. The total synthesis of (+)-dysidavarones A–C (1–3) was achieved from predysidavarone 6 in a divergent manner by a late-stage introduction of the ethoxy group, which reveals the possible source of the ethoxy group within (+)-dysidavarones A–C (1–3) and provides a late-stage modifiable route for the synthesis of dysidavarone analogs for further anti-cancer activity evaluation.
LiBr as a promising redox mediator (RM) has been applied in Li-O2 batteries to improve oxygen evolution reaction kinetics and reduce overpotentials. However, the redox shuttle of Br3− can induce the unexpected reactions and thus cause the degradation of LiBr and the corrosion of Li anode, resulting in the poor cyclability and the low round-trip efficiency. Herein, MgBr2 is firstly employed with dual functions for Li-O2 batteries, which can serve as a RM and a SEI film-forming agent. The Br– is beneficial to facilitating the decomposition of Li2O2 and thus decreasing the overpotential. Additionally, a uniform SEI film containing Mg and MgO generates on Li anode surface by the in-situ spontaneous reactions of Mg2+ and Li anode in an O2 environment, which can suppress the redox shuttle of Br3− and improve the interface stability of Li anode and electrolyte. Benefiting from these advantages, the cycle life of Li-O2 battery with MgBr2 electrolyte is significantly extended.
Carbon dots (CDs) have been extensively studied owing to their fascinating optical properties and wide potential applications. Here, we report an easy-to-perform and organic-solvent-free synthesis strategy for green-emissive CDs (G-CDs) possessing high photoluminescence (PL) quantum yield (QY). The G-CDs are synthesized by heating the homogeneous precursors of citric acid and cyanamide in an open vessel, circumventing the use of organic solvents, complex operations, high-pressure reactors, and expensive instruments in the synthesis process. The effect of various reaction variables on the formation and the optical properties of G-CDs are systematically investigated. The resultant G-CDs show bright PL emission at 521 nm with PL QY up to 73%. Then a white light-emitting diode (LED) with Commission Internationable de L'Eclairage (CIE) coordinates of (0.33, 0.34) and color rendering index (CRI) of 92 is constructed based on G-CDs/thermoplastic polyurethane (TPU) composite. Moreover, a visual microfluidic detection platform is designed by using G-CDs as fluorescent probes for rapid quantitative detection of Fe3+, Cu2+, and Mn2+ metal ions, which can realize synchronized testing of multiple samples. This study might promote the development and preparation methods of high-performance CDs with various optical applications.
The intricate correlation between multiple degrees of freedom and physical properties is a fascinating area in solid state chemistry and condensed matter physics. Here, we report a quantum-magnetic system BaNi2V2O8 (BNVO), in which the spin correlation was modulated by unusual oxidation state, leading to different magnetic behavior. The BNVO was modified with topochemical reduction (TR) to yield TR-BNVO with partially reduced valance state of Ni+ in the two-dimensional NiO6-honeycomb lattice. Accordingly, the antiferromagnetic order is suppressed by the introduction of locally interposed Ni+ and oxygen vacancies, resulting in a ferromagnetic ground state with the transition temperature up to 710 K. A positive magnetoresistance (7.5%) was observed in the TR-BNVO at 40 K under 7 T. These findings show that topological reduction is a powerful approach to engineer low-dimensional materials and accelerate the discovery of new quantum magnetism.
Peptide drugs are known for their high biological safety. However, compared with small molecule drugs, peptide drugs are easily oxidized and hydrolyzed as well as short in half-life. Herein, inspired by the long circulation of albumin in blood, we screened albumin binding peptides (ABPs) from a one-bead one-compound (OBOC) peptide library to increase the half-life of peptide drugs. Beads displaying random peptides were screened using fluorescent labeled human serum albumin. Fluorescent beads with specific binding to albumin were isolated for sequencing. The selected ABPs can effectively bind to albumin, thus possessing the long circulation of albumin. The dissociation constant (KD) of ABPs to albumin is up to 1 × 10−8 mol/L. Once one of ABPs (ABP2) was coupled to triptorelin, the circulation half-life of triptorelin in mice was significantly prolonged to 263.50 h much longer than that of triptorelin alone (179.07 h). In addition, the combination therapy using ABP-conjugated triptorelin and doxorubicin (DOX) can effectively inhibit the proliferation of tumor cells in mice. The OBOC screening strategy and resulting ABPs showed great potential for enhancing the delivery efficiency of peptide drugs.
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