Latest ArticlesThirty-one new 10,12-disubstituted aloperine derivatives were subtly constructed through a selective oxidation on the 10-α-C–H induced by sulfonyl and a nucleophilic substitution with the stereoselectivity and scalability. Of them, compound 6b displayed a moderate anti-human coronavirus OC43 (HCoV-OC43) potency and blocked the viral entry stage through a host mechanism of action. Using chemoproteomic techniques, both transmembrane serine protease 2 (TMPRSS2) and scavenger receptor class B type 1 (SR-B1) proteins, which act as host cofactors of viral entry, were identified to be the direct targets of 6b against HCoV-OC43. Furthermore, 6b may deactivate the TMPRSS2 by inducing a change in protein conformation, rather than binding to its catalytic center, thus suppressing the viral membrane fusion. Accordingly, our study provided key scientific data for the development of aloperine derivatives into a new class of antiviral candidates against human β-coronavirus, including severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2).
High-performance carbon dots (CDs) allowing the application in high-end display devices are highly desirable and usually limited by the absence of simple and easy synthesis methods. In this work, we exploited an easy-to-implement strategy for the one-step synthesis of green-emitting CDs (G-CDs) with superb optical properties. The G-CDs were synthesized using m-phenylenediamine (m-PD) as a single precursor, and the reaction reacted at 180 ℃ for 12 h The resultant G-CDs exhibit high-purity and excitation-independent green fluorescence with the photoluminescence (PL) peak located at 516 nm, full width at half maximum (FWHM) of 46 nm, and PL quantum yield (QY) of ~80% under the 470 nm excitation light. The G-CDs and corresponding composite film prepared with polyvinyl butyral (G-CDs@PVB) exhibit good PL stability after undergoing long-time storage for one year and 360 h exposure under 460 nm blue light. The G-CDs@PVB film was used as color-conversion materials in green-emitting light-emitting diode (LED) application, exhibiting a Commission internationale de l'Eclairage (CIE) chromaticity coordinate of (0.21, 0.44). The film was also used in CD-based liquid crystal display (CD-LCD) application, achieving a color gamut value of 85%. This work will offer a working basis for the synthesis of high-performance CDs as well as their application in displays.
Chiral alcohols and amines are important structural units widely existing in pharmaceuticals, agrochemicals, and food additives. Dynamic kinetic resolution (DKR) is an efficient strategy to deliver optically active alcohols and amines from their racemates. For the development of DKR method, racemization catalyst plays as a crucial element with the requirement of compatibility with the kinetic resolution (KR) system. In this paper, recent advance in the catalytic racemization of secondary alcohols and amines is summarized based on different types of racemizing intermediates, which are redox racemization via ketone/imine intermediates, racemization via radical intermediates, and racemization via carbocation intermediates. Enzymatic racemization of secondary alcohols and amines is also enclosed.
It is of great interest to make a degradable material widely tailorable to replace petroleum-derived products among diverse applications. Here, we report the construction of a new multi-purpose degradable material for the first time via a simple ternary copolymerization system comprising ε-caprolactone (ε-CL), cyclohexane oxide (CHO) and CO2. Under low pressure of 1 bar ~5 bar, the ring-opening polymerization (ROP) of ε-CL and ring-opening copolymerization (ROCOP) of CO2 and CHO can simultaneously proceed. The carbonate units are randomly distributed on the polymer chain. These random terpolymers have controllable molar mass (10–106 kDa) and compositions (4–33 mol% CO2). And the obtained materials show large-span tunability from tough plastic to elastomer and even adhesive.
Covalent adaptable networks (CANs), which share the properties of both thermosets and thermoplastics at the same time, are desirable for many applications. Introducing bulky substituents is a feasible way to design dynamic covalent bonds for constructing CANs, as evidenced by the successful implementation in CANs based on hindered urea bonds (HUBs). However, the dynamicity induced by introducing bulky substituents always come with low bond energy, resulting in low mechanical strength and poor stability of the CANs. Herein, we designed a novel hindered urethane bond, which is weak in thermodynamic (Keq = 1701.23 L/mol at 25 ℃) and inert in kinetic at low temperature, but stable in thermodynamic (Keq = 1.54 × 104 L/mol at 100 ℃) and active in kinetic at high temperature (k-1 = 0.105 h−1 at 80 ℃ and 0.315 h−1 at 120 ℃). As a result, the polyurethane based on it exhibits high mechanical properties (with Youngs' modulus of 1011 ± 29 MPa and flexible modulus reached 1833 ± 50 MPa) and excellent reversibility (can be reprocessed at 60 ℃ under 100 kPa in 30 min and completely healed at 40 ℃ in 10 min). Moreover, unlike to many CANs based on hindered urea bonds, our dynamic polyurethanes are highly stable in humid environment or even water solutions due to the slow hydrolysis kinetics. Such high-performance dynamic polyurethane polymers are attractive for many applications.
Zinc-based batteries (ZBs) have been deemed as a potential substitute for lithium-ion batteries due to its unique advantages of abundant resources, low cost and acceptable energy density. Despite great progress in designing electrode materials has been made, the development of high-performance ZBs still remain challenges, such as the dendrite growth of zinc anode, hydrogen evolution reaction, limited electrochemical stability window, water evaporation and liquid leakage. Gel polymer electrolytes (GPEs), including hydrous GPEs with low content of active water and anhydrous GPEs without the presence of water, are proposed to avoid these problems. Furthermore, employing GPEs is conductive to fabricate flexible devices owing to the good mechanical strength. To date, most of researches focus on discovering new GPEs and exploring its application on flexible or wearable devices. Recent reviews also have outlined the polymer matrixes and advances of GPEs in various battery systems. Given this, herein, we seek to summarize the gelation mechanisms of GPEs, involving physical gel of polymer, chemical crosslinking of polymer and chemical polymerization of monomers. Peculiarly, the preparation methods are also classified. In addition, not only the features and central conundrum of GPEs are analyzed but also the corresponding strategies are discussed, contributing to design GPEs with ideal properties for high-performance ZBs.
Water pollution caused by global population growth, urban expansion and industrialization development is one of the urgent issues that need to be addressed in the 21st century. Up to now, it was challenging for metal-organic frameworks (MOFs) to be used in the actual water treatment due to that the powder MOFs suffered from difficult reuse, poor water stability and easy corrosion. It is an effective strategy to immobilize MOFs powder onto porous sponge foam carriers for accomplishing large flux, facile recycling, easy processing water treatment setups. In this review article, the fabrication approaches and applications of different MOFs/sponge composites were highlighted, in which the fluorescence detection of pollutants, adsorption and separation of pollutants, catalytic reduction and oxidation of pollutants were included. Finally, the future challenges and opportunities of MOF/sponge for water treatment are proposed, aiming to provide in-depth guidance for the future design and manufacture of the immobilized MOFs onto sponge foams.
The galactomannan from Antrodia cinnamomea (AC) is characterized as one of the important bioactive components that exhibits potential immunostimulatory propriety. The biological function of its corresponding oligosaccharide fragments has not been revealed yet. In this study, we reported the first chemical synthesis of the series of oligosaccharide fragments related to AC galactomannan via the convergent glycosylation strategy. The preliminary immunological evaluation of these synthesized AC oligosaccharides disclosed that the backbone tetrasaccharide 1d showed the best immunomodulatory ability on enhancing proliferation, phagocytosis and cytokines secretion of Raw264.7 macrophages in vitro, indicating its immense potential as an immunostimulant candidate.
In September 2018, we proposed the cutting-edge concept of "Beyond Limits Manufacturing" (BLM). BLM technology is based on the three-dimensional inner engraving or precise outer engraving of ultra-fast laser, to invent micro/nano scale flow chips or devices, which makes it possible for the microform, integration, economy, safety, high efficiency, green and intelligence of research, development and manufacturing process, so as to realize transformational manufacturing in the era of Industry 4.0. In this paper, we reviewed the representative results we made in the field of micro/nano flow chemistry during the implementation of the BLM major project (December 2019 to August 2023), and discussed its application prospects in micro/nano flow chemistry.
As key biomarkers, amyloid-β (Aβ) plaques are frequently used to diagnose Alzheimer's disease (AD). Although fluorescence imaging has proven to be effective in detecting these plaques, the gold standard probe thioflavin T (ThT), used for Aβ aggregates, cannot be applied in vivo owing to its invasive nature. Therefore, the development of novel fluorescent probes capable of identifying Aβ plaques in situ is necessary. Based on the ThT structure, two π-conjugated heterocyclic D-π-A probes were designed bearing the hydroxytricyanopyrrole acceptor and N,N-dimethylaminophenyl donor. These probes exhibited red to near-infrared fluorescence emission (λmax = 732 nm), large Stokes shifts (>100 nm), exceptional signal-to-noise ratio, rapid response (<30 s), and high binding affinity (NT-HTCP = 33.32 nmol/L; NF-HTCP = 53.35 nmol/L) for Aβ aggregates. As the best candidate, NT-HTCP was used for in situ imaging of Aβ plaques in AD mouse models. Furthermore, in vivo research demonstrated that NT-HTCP could cross the blood–brain barrier and continue imaging the Aβ plaques with a good signal-to-noise ratio. Additionally, the outcomes of the docking computations helped guide the development of the Aβ probes. This study expands the family of N,N-dimethylaminophenyl-based Aβ-sensitive fluorophores, with NT-HTCP emerging as a highly promising imaging agent.
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