Latest ArticlesDeveloping applicable methods to forge linkages between sp3 and sp2-hydridized carbons is of great significance in drug discovery. We show here a new, Ni-catalyzed reductive cross-coupling reaction that forms Csp3−Csp2 bonds from aryl iodides and cyclic sulfonium salts. Notably, Csp3−Csp2 bonds can be forged selectively at the iodine-bearing carbon of bromo(iodo)arenes which is usually recognized as a huge challenge under the catalytic reductive cross-coupling (CRCC) conditions. Experimental and computational mechanistic studies support LNiⅠAr as an active species, while the untraditional anti-Markovnikov selective alkylation of asymmetric sulfonium salts is determined by the oxidative S-substitution of sulfonium salts with LNiⅠAr. This protocol further expands the range of alkyl electrophiles under the CRCC conditions and provides a new strategy for the construction of Csp3−Csp2 bonds.
Roxarsone (ROX) is a commonly used antibacterial and growth-promoting additive to animal feed. The development of an effective method for detecting ROX and its conversion products is of importance because of their potential harm to human health and ecosystem. Herein, we report the designed synthesis of a novel one-dimensional covalent organic framework (1D COF), named EP-COF, and its application as a fluorescent probe for ROX sensing. EP-COF is constructed based on imine linkages, exhibiting high crystallinity, strong fluorescence emission, and good dispersibility in water. It displays a remarkable capability to efficiently detect ROX, with an impressive detection limit of 4.5 nmol/L. Moreover, EP-COF also offers advantages of excellent selectivity, and high structural stability. This work not only presents a promising approach for the detection of harmful substances like ROX, but also serves as a valuable reference for exploring application of 1D COFs in chemical sensing.
The supramolecular Förster resonance energy transfer (FRET) is seen as a promising approach for organic photocatalysis using dyes as catalysts, because it combines the high efficiency of energy transfer with the dynamic responsiveness based on non-covalent interactions. Here we propose a supramolecular FRET photocatalysis strategy for α-oxyamination reaction based on supramolecular confinement effect. The well-designed benzothiadiazole-based cationic monomer as energy donor and the dyes of Nile Red as acceptor are doped into the amphiphilic surfactants of sodium dodecyl sulfate (SDS). Benefitting from the supramolecular confinement space provided by SDS in aqueous environment, the FRET process between the monomer and Nile Red is effectively achieved (exciton migration rate: 3.99 × 1014 L mol‒1 s‒1). On this basis, the supramolecular FRET system is used as an efficient energy source to catalyze α-oxyamination reactions between a series of 1,3-dicarbonyl compounds and 2,2,6,6-tetramethylpiperidine-1-oxyl under white LED light, showing a yield as high as 94% and a turnover frequency value of 3.92 h‒1. This photocatalytic result shows a great enhancement compared to that of Nile Red alone.
Antibiotic resistance poses a critical threat to human healthcare, largely driven by bacterial biofilms. These biofilms resist the immune system and antibiotics, rendering enclosed microbial cells 10–1000 times more antibiotic-resistant than planktonic cells, leading to severe infections. Therefore, there is an urgent need to develop innovative tools for investigating biofilm regulators and devising novel antibacterial strategies. In this study, we developed Cy-NEO-PA, a near-infrared (NIR) fluorescent probe responsive to penicillin G acylase (PGA), with bacteria-targeting ability. This probe was designed to visualize the influence of environmental factors on biofilm formation in Acinetobacter baumannii (A. baumannii). Our findings demonstrated that glucose suppressed PGA production, leading to enhanced biofilm formation, whereas phenylacetic acid (PAA) stimulated PGA production and inhibited biofilm formation in A. baumannii. These observations highlight the remarkable capability of Cy-NEO-PA to accurately measure PGA dynamics, shedding light on the critical role of PGA in biofilm development. Additionally, Cy-NEO-PA exhibited excellent biocompatibility, potent reactive oxygen species (ROS) generation, efficient photothermal conversion, and bacteria-targeting abilities, making it a promising agent for combating bacterial infections and promoting wound healing through photothermal (PTT)/photodynamic (PDT) therapy. These discoveries emphasize the significant role of PGA in antibacterial therapy and offer valuable insights for the design of effective strategies targeting PGA to combat biofilm-associated infections.
This review profiles twelve fluorine-containing drugs approved by the US Food and Drug Administration (FDA) for the clinic in 2023. These small molecule drugs represent such therapeutic areas as cancer, neuromuscular disorder, immunodeficiency, virology, and infectious diseases. Medicinal chemistry discovery, biological activity, and synthetic routes have been discussed for each drug. Also, new trends in structural positioning, functionality, and degree of fluorination are discussed. Besides fluorination, the importance of amino acid residues and chirality in the design of new pharmaceuticals is highlighted.
Reported here is the synthesis of a new macrocycle bearing anionic carboxylate groups with water-soluble aggregation-induced emission (AIE). The water-soluble macrocycle without typical AIE luminogens is constructed based on the building block of benzothiadiazole. It exhibits a remarkable AIE effect. This water-soluble macrocycle can selectively bind different types of biogenic amines in aqueous media with the tightest binding towards spermine. The fluorescence enhancement induced by supramolecular encapsulation is used to detect spermine.
The construction of enzyme reactors based on metal-organic frameworks (MOFs) as the immobilized matrix is a proven strategy that has achieved the widespread application of enzymes across industries. Although many MOFs and a variety of strategies have been developed, a formidable challenge remains in maintaining the high enzyme activity with excellent recyclability and tolerance for harsh conditions. Herein, using degradable redox stimuli-responsive liposomes as the templates with microporous MOFs (M-MOFs) as the hosts for enzyme encapsulation, a series of enzyme reactors (enzyme@M-MOFs) was designed and created. Based on the premise of enhancing enzyme protection in the harsh environment, this strategy provided a high degree-of-freedom space via removal of liposomes that improved the conformational freedom of the enzymes, promoted the mass transfer of substrates and products, and greatly boosted the catalytic activity. Importantly, the strategy had good universality and was applied to various liposomes, M-MOFs and enzymes. Additionally, the co-encapsulation of different enzymes with synergistic functions was performed using the M-MOFs platform. This study solved the problems of the conformation limitation of enzymes and mass transfer resistance of substrates and products using the proposed enzyme@M-MOFs, providing a new approach for the construction of biological cascade reaction devices based on MOFs materials.
The device configuration with mesoporous titanium dioxide (m-TiO2) has garnered considerable attention as a promising solution for high-stable perovskite and dye-sensitized solar cells, although its application in organic solar cells remains unexplored. In this communication, we have incorporated this structure into both bulk-heterojunction (BHJ) and single-component organic solar cells (SCOSCs). Surprisingly, mesoporous OSCs (M-OSCs) demonstrate a deteriorative efficiency in BHJ-type cells, whereas this configuration succeeds in SCOSCs, exhibiting competitive performance with planar OSCs (P-OSCs). This pioneering study has resulted in a competitive power conversion efficiency of 9.67% for m-TiO2-based cells, marking a significant milestone in the advancement of OSCs. Importantly, profiting from the better ultraviolet resistance of m-TiO2 than zinc oxide, this M-OSC exhibits superior photostability than that of P-OSCs when subjected to continuous one-sun (AM1.5G) illumination. In its entirety, this research not only introduces the concept of M-OSCs for the first time but also unveils a novel device architecture poised to address the long-term stability concerns within the realm of OSCs.
The design and synthesis of organic high-temperature reversible thermochromic materials is one of the difficult issues in the field of organic chromic materials. In this paper, four diacetylene monomers named DBA-PCDA, TBA-PCDA, DBE-PCDA and TBE-PCDA, each containing multiple diacetylene units, were synthesized from 10,12-pentacosadiynoic acid (PCDA) through the amidation or esterification reactions, using 4,4′-diaminobiphenyl, 1,3,5-tris(4-aminophenyl)benzene, 4,4′-dihydroxybiphenyl, and 1,3,5-tris(4-hydroxyphenyl)benzene as bridging units. The effects of functional groups that can form hydrogen bond and π-π interactions on the solid-state polymerization properties of monomers and the thermochromic properties of the corresponding PDAs were investigated. The results show that only DBA-PCDA and TBA-PCDA, which contain functional groups that can form hydrogen bonding interactions, can be polymerized under 254-nm UV irradiation. The corresponding poly(DBA-PCDA) exhibits reversible thermochromic property even heated up to 200 ℃, showing a potential application in the field of high-temperature thermal indicator above 100 ℃. This work provides a new perspective to the development of PDA with high-temperature reversible thermochromic property.
Rechargeable magnesium ion batteries (RMBs) are investigated as lithium-ion batteries (LIBs) alternatives owing to their favorable merits of high energy density, abundance and low expenditure of Mg, as well as especially non-toxic safety and low risk of dendrite formation in anodes, which endows them to be more easily assembled in electric-power vehicles for the extended application of civilian-military fields. Nevertheless, the high charge density, strong polarization effect, and slow diffusion kinetics of Mg2+ remain a large obstacle and thus enormous efforts have to be paid to mend the gap with commercial demand for cathode materials. At present, RMBs cathode materials mainly contain transition metal sulfides/oxides, polyanionic compounds and Prussian blue analogs, and several methods such as nano structuring, doping regulation and coating modification have been applied to materials design for better performance. In this paper, the current research status of RMBs cathode materials at home & abroad is arranged and summarized along with challenges of development in the future focusing on synthesis of RMBs cathode materials with high energy density as well as satisfactory cycling performance. And this analysis aims to provide reference and basis for researchers working on RMBs technology advancement.
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