Latest ArticlesNowadays, due to excellent biological and polymeric characteristics, DNA has been widely noted as an emerging building block to construct diverse materials for biosensing, in vivo imaging, drug delivery, and disease therapy. Particularly, relying on programmability, predictability, and stability of DNA, DNA walkers have opened new and exciting opportunities in modern life sciences for target detection and biological analysis, which are constructed by self-assembly of DNA or combining DNA with other nanomaterials (e.g., quantum dots, gold nanoparticles, magnetic nanoparticles, polymers). Compared with conventional nanomaterials (lanthanide-doped upconversion nanoparticles, magnetic nanomaterials, carbon dots, silicon dots, and so on), DNA walkers showed convenient modification, lower biotoxicity, excellent biocompatibility and high biostability, improving the biological application. Meanwhile, with high-speed operating efficiency and sustainable operation, DNA walkers powered by strand displacement reaction or protein enzyme/DNAzyme reaction, have highly sensitive detection and signal amplification abilities, which are applied in biosensing, material assembly and synthesis, and early cancer diagnosis. Worthily, DNA walkers could be regarded as signal amplifiers, which enhanced the signal transduction and amplified biosensor sensing signals. Herein, we systematically and comprehensively summarized the operating principles of various DNA walkers, categorized rational design of the DNA walker, and outlined the application of DNA walker in biosensors. Furthermore, the challenges and future trends of DNA walkers were discussed.
Finding suitable strategies to effectively enhance the optical properties of materials are the goal being pursued by researchers. Herein, cation-anion synergetic interactions strategy was proposed to develop two novel organic-inorganic hybrid antimony-based optical materials, (C3H5N2)SbF2SO4 (Ⅰ) and (C5H6N)SbF2SO4 (Ⅱ), which were obtained by introducing Sb3+cation containing stereochemically active lone-pair (SCALP) and organic π-conjugated cations into sulphate system. The synergistic interactions of the organic π-conjugated cations, the inorganic [SbO2F2]3− seesaw anions and the [SO4]2− distorted tetrahedra anions make their ultraviolet (UV) absorption edges approach 297 and 283 nm, respectively, and raise their birefringence up to 0.193@546 nm and 0.179@546 nm, respectively. Interestingly, although the two compounds have the same stoichiometric ratio and similar one-dimensional (1D) chain structure, they show opposite macroscopic symmetry, where the NCS compound (Ⅱ) exhibits a large second-harmonic generation (SHG) response (1.6 times that of KH2PO4). The two reported compounds are found to be promising UV optical materials in the experimental tests.
Strategic active site organization is imperative for the advancement of effective and long-lasting catalysts of oxygen reduction reactions. However, the controllable multi-active site design is a highly intricate topic for catalyst synthesis. Employing pre-trapping and post-activation strategy, Fe-N bonding structure and S, Se functionalized heteroatom are integrated into a conductive porous carbon. In this process, the nitrogen-abundant polymer 1,3,5-triformylbenzene-tris(4-aminophenyl)benzene (Tf-TAPA) adsorbs Fe3+ under the intrinsically metal anchoring ability of N atoms and simultaneously in-situ assembles long-chain thiophene-S. Subsequently, the Fe3+ is transformed into Fe-Nx moieties with the conversion of the organic chain to incompletely graphitized carbon. Furthermore, the alteration of the electronic configuration achieved through the introduction of dual-atom S and Se leads to a pronounced enhancement in catalytic efficiency. Benefitting from the Fe-Nx bonding structure, dense structural defects, and conductive carbon networks, the resultant Fe-S,Se/NCNs possesses a positive half-wave potential of 0.86 V and a 90% current retention rate, outstripping the Pt/C benchmark. Moreover, the liquid and flexible ZAB driven by Fe-S,Se/NCNs achieves large power densities of 259.7 and 164.7 mW/cm2, respectively. This study provides a new comprehension in developing an efficient and stable M-N-C oxygen electrocatalyst.
Formaldehyde (HCHO) as an indoor air pollutant released by new furniture and decorative materials is of great concern. Developing a self-cleaning device to remove HCHO is an ideal way to improve indoor air quality. In this study, a self-cleaning window with a multilayered structure constructed from fluorine-doped tin oxide/bismuth tungstate/resorcinol-formaldehyde resin (FTO/Bi2WO6/RF) has been fabricated, which is capable of degrading HCHO in natural indoor condition. The as-fabricated device could utilize the natural room light and promote the generation and transfer of the photocatalytic carriers in Bi2WO6, which subsequently delivers a good catalytic oxygen reduction efficiency in RF to produce hydrogen peroxide (H2O2). The as-synthesized H2O2 could further split into hydroxyl radicals (•OH), then oxide the HCHO molecules in the air. The present study demonstrates a novel and efficient strategy to fabricate a transparent multifunctional window for self-cleaning indoor gaseous pollutants, the concept is of great importance to be expanded in a broad range of indoor furniture for in-house air pollution control.
Exosomes (EXOs) have showed great potential in regenerative medicine. The separation of EXOs from complex biological media is essential for the down-stream applications. Herein, we report a deoxyribonucleic acid (DNA)-based micro-complex (DMC) containing polyaptamers, which realized the specific separation of EXOs from cell culture media and the significant promotion of wound healing. The synthesis of DMCs was based on a biomineralization process via rolling circle amplification (RCA) under the catalysis of phi29 DNA polymerase. To endow DMCs with the ability to capture EXOs, the DNA template of RCA was integrated with complementary sequence of aptamer that specifically recognized the CD63 proteins on EXOs. The obtained DMCs contained polyaptamers that can specifically capture the EXOs in cell culture media. The EXOs-capturing DMCs were collected by centrifugation, achieving the separation of EXOs. Mesenchymal stem cell (MSC)-derived EXOs (MSC-EXOs) were separated by this DMC-based strategy, and the separated MSC-EXOs significantly enhanced the migration ability of cells. In particular, the significant therapeutic efficacy of the DMCs with MSC-EXOs was verified in full-thickness wound excision mouse models, in which the wounds completely healed in 10 days. We envision that this DMC-based separation strategy can be a promising route to promote the development of EXOs in biomedicine.
Carbon monoxide (CO) is a vital intracellular gas messenger known for its cytoprotective and homeostatic properties. It plays a pivotal role in a myriad of biological processes. Therefore, the precise detection of CO is of paramount importance in unraveling the intricacies of pathological mechanisms and advancing the development of disease diagnosis. We herein introduce NFCOP, a state-of-the-art near-infrared (NIR) turn-on fluorescence (FL) probe that has been meticulously designed for highly sensitive, swift and selective imaging of CO. The NFCOP response occurred rapidly with CO, within just 10 s, and the calculated detection limit for CO was determined to be 0.32 µmol/L. Further investigations conducted at the cellular level and in vivo demonstrated that NFCOP possesses high sensitivity and selectivity for imaging CO.
Nicotinamide phosphoribosyl transferase (NAMPT) is considered as a promising target for cancer therapy to its crucial role in cancer metabolism. Despite the therapeutic potential of NAMPT enzymatic inhibitors, their effectiveness is limited by dose-related toxicity and the inability to suppress nonenzymatic functions of extracellular NAMPT (eNAMPT). Herein, we designed and synthesized the first hydrophobic tagging NAMPT degraders. Among them, compound NH-11 selectively degraded NAMPT in leukemia cells through the ubiquitin-proteasome system. Compound NH-11 effectively induced apoptosis and showed low toxicity to normal cells, representing a promising anti-leukemia lead compound.
In the quest for new agrochemicals and pharmaceuticals, chemists seek access to reliable and mild synthetic techniques to allow for the systematic modification of chemical structures, exploration of unexplored chemical space, and facilitation of practical synthesis in their search for novel agrochemicals and pharmaceuticals. In this regard, photocatalytic reactions enabled the synthesis of intricate and more functionalized compounds. This review overviews the developed synthetic methodologies and their utility in the chemical synthesis of pharmaceuticals. This review also offers in-depth insights into contemporary photoredox reactions such as allylic additions, cyclization, reductive cross-coupling, CH activation, ring opening, oxidative cross-coupling, dehydrogenation, desulphonation, and decarboxylation. It provides a positive outlook for the promising future of this field.
Stimuli-triggered release and alleviating resistance of iridium(Ⅲ)-based drugs at tumor sites remains challengeable for clinical hepatoma therapy. Herein, a doxorubicin@iridium-transferrin (DOX@Ir-TF) nanovesicle was synthesized by carboxylated-transferrin (TF) and doxorubicin-loaded amphiphilic iridium-amino with quaternary ammonium (QA) groups and disulfide bonds. The QA groups enhanced photophysical properties and broadened production capacity of photoinduced-reactive oxygen species (ROS), while the disulfide-bridged bonds regulated oxidative stress levels through reacting with glutathione (GSH); simultaneously, modification of TF improved recognition and endocytosis of the nanovesicle for tumor cells. Based on in-vitro results, a controlled-release behavior of DOX upon a dual-responsiveness of GSH and near-infrared ray (NIR) irradiation was presented, along with high-efficiency generation of ROS. After an intravenous injection, the nanovesicle was targeted at tumor sites, realizing TF-navigated photoacoustic imaging guidance and synergistic chemotherapy-photodynamic therapy under NIR/GSH stimulations. Overall, newly-synthesized DOX@Ir-TF nanovesicle provided a potential in subcutaneous hepatocellular carcinoma therapy due to integrations of targeting delivery, dual-stimuli responsive release, synergistic therapy strategy, and real-time monitoring.
On-surface Ullmann-type reaction, or the dehalogenated coupling, is arguably the most pivotal reaction in on-surface synthesis for the fabrications of carbon nanostructures. Hitherto, the vast majority of works rely on activating the C-Br bond of aryl bromide which has a moderate bond dissociation energy. The C-Cl bond of aryl chloride has a higher dissociation energy and requires much higher thermal energy to break the bond. In this study, we have explored the on-surface photo-induced dechlorination and achieved the activation of three distinct aryl chlorines on the Au(111) surface with mild temperatures. This work enriches our understanding of on-surface photo-induced reactions and highlights the potential of photochemistry in realizing unconventional reactions.
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