There is a great demand to understand cell transplantation, migration, division, fusion, and lysis. Correspondingly, illuminant object-labeled bioprobes have been employed as long-term cellular tracers, which could provide valuable insights into detecting these biological processes. In this work, we designed and synthesized a fluorescent polymer, which was comprised of hydrophilic N-isopropylacrylamide polymers as matrix and a hydrophobic tetraphenylethene (TPE) unit as AIE-active cross-linkers (DDBV). It was found that when the feed molar ratio of N-isopropylacrylamides to cross-linkers was 22:1, the produced polymers demonstrated the desirable LCST at 37.5 °C. And also, the temperature sensitivity of polymers could induce phase transfer within a narrow window (32-38 °C). Meanwhile, phase transfer was able to lead the florescent response. And thus, we concluded that two responses occur when one stimulus is input. Therefore, the new cross-linker of DDBV rendered a new performance from PNIPAm and a new chance to create new materials. Moreover, the resulted polymers demonstrated very good biocompatibility with living A549 human lung adenocarcinoma cells and L929 mouse fibroblast cells, respectively. Both of these cells retained very active viabilities in the concentration range of 7.8-125 μL/mg of polymers. Notably, P[(NIPAm)22-(DDBV)1] (P6) could be readily internalized by living cells with a noninvasive manner. The cellular staining by the fluorescent polymer is so indelible that it enables cell tracing for at least 10 passages.
Electrochemical CO 2 reduction enables the conversion of intermittent renewable energy to value-added chemicals and fuel, presenting a promising strategy to relieve CO 2 emission and achieve clean energy storage. In this work, we developed nanosized Cu 2 O catalysts using the hydrothermal method for electrochemical CO 2 reduction to alcohols. Cu 2 O nanoparticles (NPs) of various morphologies that were enclosed with different crystal facets, named as Cu 2 O-c (cubic structure with (100) facets), Cu 2 O-o (octahedron structure with (111) facets), Cu 2 O-t (truncated octahedron structure with both (100) and ( 111) facets), and Cu 2 O-u (urchin-like structure with (100), ( 220), and ( 222) facets), were prepared by regulating the content of a polyvinyl pyrrolidone (PVP) template. The electrochemical CO 2 reduction performance of the different Cu 2 O NPs was evaluated in the CO 2 -saturated 0.5 M KHCO 3 electrolyte. The as-synthesized Cu 2 O nanostructures were capable of reducing CO 2 to produce alcohols including methanol, ethanol, and isopropanol. The alcohol selectivity of the different Cu 2 O NPs followed the order of Cu 2 O-t < Cu 2 O-u < Cu 2 O-c < Cu 2 O-o (with the total Faradaic efficiencies of alcohol products of 10.7, 25.0, 26.2, and 35.4%). The facet-dependent effects were associated with the varied concentrations of oxygen-vacancy defects, different energy barriers of CO 2 reduction, and distinct Cu−O bond lengths over the different crystal facets. The desired Cu 2 O-o catalyst exhibited good reduction activity with the highest partial current density of 0.51 mA/cm 2 for alcohols. The Faradaic efficiencies of alcohol products were 4.9% for methanol, 17.9% for ethanol, and 12.6% for isopropanol. The good electrochemical CO 2 reduction performance was also associated with the surface reconstruction of Cu 2 O, which endowed the catalyst with abundant Cu 0 and Cu + sites for promoted CO 2 activation and stabilized CO* adsorption for enhanced C−C coupling. This work will provide a new route for enhancing the alcohol selectivity of nanostructured Cu 2 O catalysts by crystal facet engineering.
Four cadmium and cobalt coordination polymers with unique structures and topologies have been successfully synthesized under solvothermal conditions by employing an elongated triangular rigid N-containing ligand tris(4-(1H-imidazol-1-yl)phenyl)amine (TIPA) and 5-hydroxyisophthalic acid (5-OH-H 2 bdc) as anion coligand. Compounds 1-4 were characterized by single crystal X-ray structure analyses, thermogravimetric analyses, SHG, and photoluminescent measurements. Compound 1 crystallizes in the chiral space group C2 (No. 5) and features a 2D f 3D parallel/parallel inclined polycatenated framework. Compound 2 crystallizes in trigonal symmetry with a high-symmetry space group R3 and features a 2D porous noninterpenetrating coordination network. Compound 3 crystallizes in the monoclinic space group P2 1 /n and shows a 2D f 3D parallel/parallel polycatenation framework, and compound 4 crystallizes in the orthorhombic chiral space group P2 1 2 1 2 1 (No. 19) and shows a very rarely 3D þ 3D heterogeneous 2-fold interpenetration framework built from (3,5)-connected (4 2 3 6 5 3 8 3 )(4 2 3 6) AFUQOH nets and (3,5)-connected ( 63 )(6 9 3 8) gra nets.
Solvothermal reactions of tetrakis(4-pyridyloxymethylene)methane (TPOM) with deprotonated 1,4-benzenedicarboxylate (H2bdc) or 5-hydroxyisophthalic acid (5-OH-H2bdc) in the presence of nitrates of cadmium, zinc, and cobalt in H2O or H2O/DMF produced five new complexes, namely, {[Cd2(TPOM)(bdc)2]·(H2O)5(DMF)} n (1), {[Zn2(TPOM)(bdc)2]·(H2O)4} n (2), {[Zn2(TPOM)(bdc)2]·(H2O)} n (3), {[Co2(TPOM)(5-OH-bdc)2(H2O)2]·(H2O)5} n (4), and {[Cd2(TPOM)(5-OH-bdc)2]·(H2O)2} n (5). These complexes were characterized by elemental analysis, IR spectroscopy, and X-ray single-crystal diffraction. Complex 1 reveals a 2-fold interpenetrating three-dimensional (3D) framework with pcu topology constructed from binuclear Cd clusters and TPOM ligands. In addition, the experiment of single-crystal-to-single-crystal (SC-SC) structural transformations upon guest exchange was tested. Zn complexes 2 and 3 possess different 3D frameworks and are prepared from TPOM and H2bdc under different reaction conditions. In complexes 4 and 5, TPOM and 5-OH-H2bdc link Co or Cd centers to generate 3D interpenetrating frameworks with bbf and qtz topology. In addition, thermal stabilities and photochemical properties of these new complexes in the solid state have been studied.
This is a repository copy of Seawater carbon and strontium isotope variations through the late Ediacaran to late Cambrian in the Tarim Basin.
Poor charge separation is the main factor that limits the photocatalytic hydrogen generation efficiency of organic conjugated polymers. In this work, a series of linear donor–acceptor (D–A) type oligomers are synthesized by a palladium‐catalyzed Sonogashira–Hagihara coupling of electron‐deficient diborane unit and different dihalide substitution sulfur functionalized monomers. Such diborane‐based A unit exerts great impact on the resulting oligomers, including distinct semiconductor characters with isolated lowest unoccupied molecular orbital (LUMO) orbits locating in diborane‐containing fragment, and elevated LUMO level higher than water reduction potential. Relative to A‐A type counterpart, the enhanced dipole polarization effect in D–A oligomers facilitates separation of photogenerated charge carriers, as evidenced by notably prolonged electron lifetime. Owing to π–π stacking of rigid backbone, the oligomers can aggregate into an interesting 2D semicrystalline nanosheet (≈2.74 nm), which is rarely reported in linear polymeric photocatalysts prepared by similar carbon–carbon coupling reaction. Despite low surface area (30.3 m2 g−1), such ultrathin nanosheet D–A oligomer offers outstanding visible light (λ > 420 nm) hydrogen evolution rate of 833 µmol g−1 h−1, 14 times greater than its A‐A analogue (61 µmol g−1 h−1). The study highlights the great potential of using boron element to construct D–A type oligomers for efficient photocatalytic hydrogen generation.
Within the interior of the Yangtze Craton, the dome‐like Huangling anticline exposes ca. 1000 km2 of Archaean basement and Neoproterozoic granitoid rocks in the Three Gorges region, providing a natural laboratory for studying the mechanism of intracontinental exhumation. Cretaceous shortening of the Qinling Orogen and Cenozoic reorganization of the Yangtze River have been considered by previous thermochronology studies to account for the two‐phase exhumation of the Huangling anticline. However, little is known about when and how the batholithic rocks were exposed to the surface. To fully reveal the exhumation history of the Huangling anticline, we focus on the Cenozoic sedimentary record in the western Jianghan Basin, downstream of the Three Gorges, and examined spatio‐temporal changes in sedimentation dynamic and provenance on the basis of sedimentary facies, palaeocurrents and clast compositions, as well as zircon U‐Pb geochronology. Our results indicate continuous unroofing of the Huangling anticline since the Eocene and provide a solid evidence for first exposure of the Huangling batholith during the Neogene. Cenozoic exhumation of the Huangling anticline is synchronous with incision of the Three Gorges, indicating a mechanism of intracontinental exhumation due to Yangtze River reorganization through which the Middle Yangtze River was progressively captured by the Lower Yangtze River with locally increased erosion rates in the Three Gorges.
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