Latest ArticlesIntracellular ATP is an emerging biomarker for cancer early diagnosis because it is a key messenger for regulating the proliferation and migration of cancer cells. However, the conventional ATP biosensing strategy is often limited by the undesired on-target off-tumor interference. Here, we reported a novel strategy to design enzymatically controlled DNA tetrahedron nanoprobes (En-DT) for biosensing and imaging ATP in tumor cells. The En-DT was designed via rational engineering of structure-switching aptamers with the incorporation of an enzyme-activatable site and further conjugation on the DNA tetrahedron. The En-DT could be catalytically activated by apurinic/apyrimidinic endonuclease 1 (APE1) in cancer cells, but they did not respond to ATP in normal cells, thereby enabling cancer-specific ATP biosensing and imaging in vitro and in vivo with improved tumor specificity. This strategy would facilitate the precise detection of a broad range of biomarker in tumors and may promote the development of smart probes for cancer diagnosis.
Owing to the serious potential side-effects on the environment and human health, the rapid detection and removal of antibiotics have become an important research focus. In this work, four zinc-based metal-organic frameworks (MOFs) with different functional groups, i.e., Zn-MOF, Zn-MOF-CH3, Zn-MOF-NO2, Zn-MOF-COOH, were utilized for the construction of LDO/MOF composite materials with a nickel-iron-cobalt-based layered double oxide, NiFeCo-LDO. The results showed that the LDO/MOF composites not only had high sensitivity in detecting sulfonamide and quinolone antibiotics, but also had an appreciable ability to adsorb them from wastewater. The maximum adsorption capacities of all the four types of LDO@Zn-MOFs to all antibiotics can at least reach 150 mg/g, and the limits of detection in relation to all four antibiotics were at least as low as 100 µg/L. Our work suggested the dual-function extraction performance can be attributed to the synergistic effects between the LDO and the MOFs. Moreover, the strong ferromagnetism derived from the LDO provided great convenience for the separation and regeneration of the LDO/MOF composites.
The dynamic kinetic asymmetric transformation of racemic propargylic ammonium salts with prochiral aldimine esters through a stereodivergent propargylation is catalyzed by dual nickel and copper catalysis. Thus, a diverse range of optically active α-quaternary amino esters were produced via CN bond cleavage with high reaction efficiency and stereoselectivity (up to > 99% ee). By selection of the appropriate pairwise combination of catalyst configurational isomers, all four possible stereoisomers of the corresponding propargylation products are obtained in high yields with excellent regio-, diastereo-, and enantioselectivities.
This study presents an unexpected finding that the cis isomer of β-thio-Asp exhibits higher ligation activity than the trans isomer. This discovery sheds light on the intricate nature of native chemical ligation and highlights the importance of factors beyond the steric effects of the side chain in modulating ligation activity.
The advancement of energy storage technology has paved the way for the application of electrochemical processes in achieving low-carbon and precise environmental pollution reduction. Electrodes play a crucial role in efficiently removing organic pollutants and heavy metals. To implement electrochemical pollution control technology in practical engineering, flexible electrode preparation is vital. This review highlights recent progress in flexible electrode research, focusing on the selection and structural design of flexible electrode materials. It summarizes the latest advancements in current collectors, active materials, and preparation methods to enhance conductivity, flexibility, and cycle stability. The application of flexible electrodes in water pollution control is categorized into three aspects: Organic pollutants, inorganic pollutants, and composite pollutants. Finally, the challenges and research requirements for enhancing electrode flexibility in environmental governance are discussed, along with prospects for their future applications.
Metal-nanocluster materials have gradually become a promising electrode candidate for supercapacitor application. The high-efficient and rational architecture of these metal-nanocluster electrode materials with satisfied supercapacitive performance are full of challenges. Herein, Fe-nanocluster anchored porous carbon (FAPC) nanosheets were constructed through a facile and low-cost impregnation-activation strategy. Various characterization methods documented that FAPC nanosheets possessed a mesopore-dominated structure with large surface area and abundant Fe-N4 active sites, which are crucial for supercapacitive energy storage. The optimal FAPC electrode exhibited a high specific capacitance of 378 F/g at a specific current of 1 A/g and an excellent rate capability (271 F/g at 10 A/g), which are comparable or even superior to that of most reported carbon candidates. Furthermore, the FAPC-based device achieved a desired specific energy of 14.8 Wh/kg at a specific power of 700 W/kg. This work opens a new avenue to design metal-nanocluster materials for high-performance biomass waste-based supercapacitors.
Heterocycle-braced cyclic peptides have demonstrated enhanced metabolic stability, increased potency and selectivity. Here, we present a rapid synthesis method for constructing Trp(C7)-alkene(E)-crosslinked cyclic peptides with potent anti-proliferative activities against cancer cells, through C-H alkenylation and macrolactamization. This report addresses critical challenges associated with the installation and removal of the directing group N-Piv, configuration selectivity of the olefin, and intramolecular cyclization. Notably, this method exhibits mild reaction conditions, traceless removal of the directing group, and high configuration selectivity.
The development of low-cost, earth-abundant and environmentally benign transition metal catalysts, which can catalyze multiple different types of asymmetric reactions, is an important objective in modern asymmetric catalysis. Herein we demonstrate that a chiral Ni/P-Phos catalyst achieves three types of asymmetric reactions: allenylic substitution of racemic allenic ethers, 1,4-hydroalkylation of prochiral 1,3-enynes and double alkylation of newly designed enynyl ether reagents. Three methods complement each other and produce various axially chiral allene derivatives bearing a pyrazolidine-3,5-dione unit, which is widely present in drugs and biologically active molecules with versatile pharmacological activities.
The atom-economical C-F insertion chemistry is emerged as a promising technology for the synthesis of various fluorinated scaffolds, which have wide applications both in the academic and the industrial communities. The past three years have witnessed rapid developments in this field. This highlight provides an overview on the evolution according to the fluorinating agents used.
A photochromic molecular rotor based on stiff-stilbene (SSB-FMR) was handily prepared through coupled reaction, and further self-assembled with cucurbit[8]uril (CB[8]) to form a 2:2 quaternary supramolecular complex (SSB-FMR/CB[8]). Significantly, the intervention of CB[8] on SSB-FMR achieved dual functions that assembly-induced emission enhancement and assembly-induced improvement of photoisomerized performance (especially reversibility) of stiff-stilbene molecular photoswitch. The supramolecular strategy further facilitated the assembly as a photoresponsive fluorescence switch with outstanding fatigue resistance, which was expediently applied in high-security-level QR code anti-counterfeiting and controllable lysosome targeted imaging. The study unprecedentedly provides a supramolecular method for highly efficiently improving photoisomerized performance especially reversibility of molecular photoswitches based on stiff-stilbene, and is of vital significance for the construction of intelligent materials with excellent capability.
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