【最新中稿作品】超疏水表面、光催化、生物传感核酸、肿瘤免疫等-科技论文配图-医学动画-动画宣传片-三维机械动画制作-北京中科幻彩

Endowing artificial advanced materials and systems with biomimetic self-regulatory intelligence is of paramount significance for the development of somatosensory soft robotics and adaptive optoelectronics. Herein, a bioinspired 2,4,6-Triphenylpyrylium (TPT+) functions as a classic organic photocatalyst and exhibits a noteworthy absorption in the visible range, strongly oxidizing excited states, and a somewhat unstable structure. Inspired by the nuclear chromophore and dual catalysis strategy, herein, we report a universal photoredox platform constructed by TPT+-mimic bridging ligands and reductive metal ions on the basis of metal–organic supramolecular systems for various organic couplings and molecular oxygen activation under visible-light irradiation. Significant photoinduced electron transfer and ligand-to-metal charge-transfer events are both integrated and regulated by the spatial and kinetic confinement effects of the structurally confined microenvironments, effectively improving the efficiency of electron transfer and radical–radical coupling processes in photocatalysis. This package deal provides a promising way for the design of novel photocatalysts and the development of versatile and sustainable synthetic chemistry. phototropism like a hollow stem of plants in nature. As a proof-of-concept demonstration, an adaptive photovoltaic system with solar energy harvesting maximization is illustrated. This work can provide insights into the development of artificial intelligent materials toward adaptive optoelectronics, intelligent soft robotics, and beyond.

Molecular recognition at the biointerface plays a critical role in sensing molecular interactions (e.g., DNA hybridization) and extracellular changes, which can directly affect the detection performance of biosensors (e.g., sensitivity, specificity, and response dynamics). However, conventional sensing biointerfaces show low molecular recognition efficiency due to limited target accessibility. Engineering sensing biointerfaces to regulate the orientation, spacing, and density of surface-confined molecular probes offer an effective approach to improve molecular recognition at interfaces. Over the last decades, biointerface engineering with nucleic acid materials has advanced the fundamental understanding of DNA hybridization kinetics and facilitated the design of improved biosensing platforms for monitoring cellular activities and diagnosing relevant diseases. This review summarizes the recent progress in nucleic acid-based biointerface engineering. The development of nucleic acid materials that can be applied to specific diagnostic applications is briefly introduced. Then the roles of nucleic acids in tailoring the properties of nanosurfaces, cell surfaces, and macroscopic surfaces are discussed and their biosensing applications are comprehensively highlighted. Finally, future challenges and perspectives of emerging technologies and applications in the field are presented.

Immune checkpoint blockade (ICB) therapy has revolutionized clinical oncology. However, the efficacy of ICB therapy is limited by the ineffective infiltration of T effector (Teff) cells to tumors and the immunosuppressive tumor microenvironment (TME). Here, we report a programmable tumor cells/Teff cells bispecific nano-immunoengager (NIE) that can circumvent these limitations to improve ICB therapy. The peptidic nanoparticles (NIE-NPs) bind tumor cell surface α3β1 integrin and undergo in situ transformation into nanofibrillar network nanofibers (NIE-NFs). The prolonged retained nanofibrillar network at the TME captures Teff cells via the activatable α4β1 integrin ligand and allows sustained release of resiquimod for immunomodulation. This bispecific NIE eliminates syngeneic 4T1 breast cancer and Lewis lung cancer models in mice, when given together with anti-PD-1 antibody. The in vivo structural transformation-based supramolecular bispecific NIE represents an innovative class of programmable receptor-mediated targeted immunotherapeutics to greatly enhance ICB therapy against cancers.

The palladium-catalyzed borylative cyclization via C—H activation has been developed. By this chemistry, the indole-fused dihydro-pyrrole motif, which is a kind of important unit in natural products and bio-active molecules, could be constructed and installed with a boric ester group. Furthermore, the utilities of products have been illustrated by the study of further transformations. Importantly, by using chiral ligand, the enantioselectivity of this borylative cyclization reaction could be controlled. Moreover, the borylative mechanism, which should proceed through a Pd(II)/Pd(IV) catalytic cycle, has been proposed based on the DFT calculations.

Ethanol as a fuel additive and energy carrier has been received much attention recently due to the importance of carbon neutralization and reduction of carbon emissions. The current ethanol product strongly relies on grain fermentation, which competes with human food. The conversion of syngas (a mixture of CO and H2) to ethanol has provided an alternative route that avoids competition with food. In this process, rhodium nanoparticle catalysts have exhibited unique catalytic properties, but there is still a gap in meeting the demand. The performances of these catalysts are strongly related to the geometric and electronic structures of the Rh species, where the controlled cleavage of C–O in CO, hindered deep hydrogenation to methane, and selective C–C coupling to ethanol are highly desirable. This review discusses the reaction mechanism of Rh-catalyzed ethanol production from syngas and summarizes the recent progress in Rh catalysts related to improving catalytic activity, ethanol selectivity, and durability. Based on these results, the structure-performance interplay of rhodium-based catalysts is briefly concluded. Particularly, zeolite-fixed Rh-based nanoparticles are highlighted, which might guide the development of more efficient catalysts via Rh-zeolite synergism.