Latest ArticlesA new, four component copper(Ⅰ)-catalyzed interrupted click/radical relay cascade has been developed. This unprecedented interrupted click reaction provides a rapid modular synthesis of triazole sulfones, important privileged heterocyclic pharmacophores which cannot be accessed by a traditional click reaction. Radical interception of cuprate-triazole, the key reaction intermediate formed in situ, is an important feature of this process.
Bare Pd metal nanoparticles invariably suffer from poor selectivity in furfural hydrogenation by forming flat configurations, with the aromatic ring of the substrate molecules parallel to the metal surface. Herein, we put forward a promising solution by using CeO2 as promoters to modify Pd nanoparticles for modulating the adsorption behaviors of furfural molecules. To achieve the highly-desired ultra-small Pd@CeO2 core@shell nanostructure, a "constrained auto-redox" synthesis is developed, in which silicalite-1 supports play the key role of providing their surface as the landing place of PdOx precursors for inhibiting the overgrowth and the deformation. To the best of our knowledge, this is one of the smallest core@shell materials obtained from aqueous synthesis. When evaluated as catalysts, Pd@CeO2/S-1 gives 98.9% conversion of furfural with 94.3% selectivity for furfural alcohol in 15 h, which is much better than that of Pd/S-1 (88.6% conversion with 44.3% selectively). The DFT simulation reveals a strong interaction between the defects of CeO2 and the oxygen atom of the –CHO group in furfural molecules, which benefits the selective hydrogenation occurred in the –CHO group rather than the furan ring.
Flexible aqueous zinc-ion batteries (AZIBs) with air-recharging capability are a promising self-powered system applied in future wearable electronics. It is desired to develop high-capacity air-rechargeable AZIBs. Herein, we developed a flexible AZIB with air-recharging capability based on trinitrohexaazatrinaphthylene (TNHATN) cathode and a ZnSO4 electrolyte. The flexible Zn//TNHATN battery exhibits high volumetric energy density (21.36 mWh/cm3) and excellent mechanical flexibility. Impressing, the discharged flexible Zn//TNHATN battery can be chemical self-charged via the redox reaction between TNHATN cathode and O2 from the air. After oxidation in air for 15 h, such flexible Zn//TNHATN battery can deliver a high specific capacity of 320 mAh/g at 0.5 A/g, displaying excellent air-recharging capability. Notably, this flexible Zn//TNHATN battery also works well in chemical or/and galvanostatic charging mixed modes, showing reusability. This work provides a new insight for designing flexible aqueous self-powered systems.
An inexpensive phosphine catalyst was used effectively for a transition-metal-free acyl-transfer of N-containing heteroaryl ketones for the rapid synthesis of N-fused heterocycles. The key pre-aromatic spirocyclic intermediate initialized by the single electron transfer (SET) process of Togni's reagent Ⅱ promoted by the tertiary phosphine resulted in an intriguing and alternative tactic for the cleavage of C‒C bonds. By using inexpensive tertiary phosphine as the catalyst, this skeleton-reorganizing approach of N-containing heteroaryl ketones allows a streamlined assembly of complex N-fused heterocycles with broad functional group tolerance.
Fabrication of single atom catalysts (SACs) by a green and gentle method is important for their practical Fenton-like use. In this work, a high effective iron-based catalyst was prepared from the iron-rich Enteromorpha for NPX degradation via peroxymonosulfate (PMS). Both Fe-SACs and iron-clusters was fabricated from the intrinsic iron element in Enteromorpha after the urea saturation. The Fe-SACs/clusters can achieve 100% of NPX oxidation within 20 min with the kobs of 0.282 min−1. Quenching tests indicated that the radical pathways were not dominated in the catalytic systems, and strong electron transfer process can be induced in the Fe-SACs/clusters + PMS system by using the NPX as electron donor and Fe-SACs/clusters/PMS* complexes as electron acceptor. This result was consistent with the phenomenon observed in the galvanic oxidation system. In addition, the Fe-SACs/clusters was deposited onto the ceramic membrane (CM) by the spraying-crosslinking process to form a Fe-SACs/clusters@CM, which showed an effective and continuous NPX degradation in a heterogeneous PMS system.
The pharmaceutical industry is now paying increased attention to continuous manufacturing. While the revolution to continuous and automated manufacturing is deepening in most of the top pharma companies in the world, the advancement of automated pharmaceutical continuous manufacturing in China is relatively slow due to some key challenges including the lack of knowledge on the related technologies and shortage of qualified personnels. In this review, emphasis is given to two of the crucial technologies in automated pharmaceutical continuous manufacturing, i.e., process analytical technology (PAT) and self-optimizing algorithm. Research work published in recent 5 years employing advanced PAT tools and self-optimization algorithms is introduced, which represents the great progress that has been made in automated pharmaceutical continuous manufacturing.
A meso-molecular muscle was prepared by capping the [c2]daisy chain based on a mono-functionalized copillar[5]arene with an imidazolium group in its axle. From its crystal structure, we observed that it was a cyclic dimer composed of two mirror image subcomponents, a pR- and a pS-copillar[5]arene. Their conformations were fixed by the doubly interlocked mechanical bond. By comparison of the 1H NMR and COSY spectra, we found that the length of this meso-molecular muscle could be controlled not only by the solvents, but also by the counter anions.
Organic electrochemical transistors (OECTs) have emerged as one type of promising building block for neuromorphic systems owing to their capability of mimicking the morphology and functions of biological neurons and synapses. Currently, numerous kinds of OECTs have been developed, while self-healing performance has been neglected in most reported OECTs. In this work, the OECTs using self-healing polymer electrolytes as dielectric layers are proposed. Several important synaptic behaviors are simulated in the OECTs by doping the channel layers with ions from the electrolytes. Benefitting from the dynamic hydrogen bonds in the self-healing polymer electrolytes, the OECTs can successfully maintain their electrical performance and the ability of emulating synaptic behaviors after self-healing compared with the initial state. More significantly, the sublinear spatial summation function is demonstrated in the OECTs and their potential in flexible electronics is also validated. These results suggest that our devices are expected to be a vital component in the development of future wearable and bioimplantable neuromorphic systems.
The outbreak of COVID-19 has drawn great attention around the world. SARS-CoV-2 is a highly infectious virus with occult transmission by many mutations and a long incubation period. In particular, the emergence of asymptomatic infections has made the epidemic even more severe. Therefore, early diagnosis and timely management of suspected cases are essential measures to control the spread of the virus. Developing simple, portable, and accurate diagnostic techniques for SARS-CoV-2 is the key to epidemic prevention. The advantages of point-of-care testing technology make it play an increasingly important role in viral detection and screening. This review summarizes the point-of-care testing platforms developed by nucleic acid detection, immunological detection, and nanomaterial-based biosensors detection. Furthermore, this paper provides a prospect for designing future highly accurate, cheap, and convenient SARS-CoV-2 diagnostic technology.
Mannich-type reactions are a widely used method for the synthesis of amines due to the readily availability of nucleophiles and electrophiles. However, the inclusion of alkylarenes instead of active carbon pronucleophiles such as aldehydes and ketones in these addition reactions has been a challenge due to the inherent difficulty of benzylic deprotonation. In this study, we present a novel approach for the construction of N-sulfonyl amines via rhodium-catalyzed addition of unbiased benzylic CH bonds to cyclic N-sulfonyl ketamines through π-coordination. This strategy enables the synthesis of a diverse range of N-sulfonyl amines, and subsequent diversification of the addition products showcases the synthetic potential of this protocol.