Laser point clouds are commonly affected by Gaussian and Laplace noise, resulting in decreased accuracy in subsequent surface reconstruction and visualization processes. However, existing point cloud denoising algorithms often overlook the local consistency and density of the point cloud normal vector. A feature map learning algorithm which integrates point normal constraints, Dirichlet energy, and coupled orthogonality bias terms is proposed.
View Article and Find Full Text PDFIn this study, the cooling effect below ambient air temperature, heat dissipation properties and heating energy efficacy of a superomniphobic self-cleaning (SSC) highly emissive (HE) coating were systematically investigated. Except at midday, the SSC-HE coating with an extremely high solar reflectance of 0.985 showed a better cooling effect than a 10-cm-thick polyurethane insulation layer.
View Article and Find Full Text PDFRecent years have witnessed marked progress in the efficient synthesis of various enantioenriched 1,2,3,4-tetrahydroquinoxalines. However, enantio- and diastereoselective access to trans-2,3-disubstituted 1,2,3,4-tetrahydroquinoxalines remains much less explored. Herein we report that a frustrated Lewis pair-based catalyst generated via in situ hydroboration of 2-vinylnaphthalene with HB(C F ) allows for the one-pot tandem cyclization/hydrosilylation of 1,2-diaminobenzenes and 1,2-diketones with commercially available PhSiH to exclusively afford trans-2,3-disubstituted 1,2,3,4-tetrahydroquinoxalines in high yields with excellent diastereoselectivities (>20 : 1 dr).
View Article and Find Full Text PDFNebulized lipid nanoparticles (LNPs) have been considered as potential therapies for genetic disease as well as infectious disease. However, the sensitivity of LNPs to high shear stress during the nebulization process results in loss of the integrity of the nanostructure and the capability of delivering active pharmaceutical ingredients. Herein we have provided a fast extrusion method to prepare liposomes incorporated with a DNA hydrogel (hydrogel-LNPs) to improve the stability of the LNPs.
View Article and Find Full Text PDFMechanical interactions between cells and extracellular matrix (ECM) are critical for stem cell fate decision. Synthetic models of ECM, such as hydrogels, can be used to precisely manipulate the mechanical properties of the cell niche and investigate how mechanical signals regulate the cell behavior. However, it has long been a great challenge to tune solely the ECM-mimic hydrogels' mechanical signals since altering the mechanical properties of most materials is usually accompanied by chemical and topological changes.
View Article and Find Full Text PDFBy combining DNA nanotechnology and solid-phase nanopore technology, the aggregation behavior of polymer guided by a single-molecular poly(propylene) (PPO) nucleus in a 3D DNA network has been studied. At low temperature, the PPO chain is evenly dispersed in the rigid 3D DNA network; at higher temperature, the PPO chain self-collapses to a single-molecular nucleus; and upon addition of amphiphilic block copolymers below the critical micelle concentration (CMC), the chains tend to aggregate on the isolated hydrophobic nucleus through intermolecular hydrophobic interactions. The process has been characterized by a rheological test and an electrochemical test.
View Article and Find Full Text PDFA Rh(I)-catalyzed trideuteromethylation of heteroarenes with inexpensive and readily available deuterated acetic acid (CDCOD) with the aid of a -containing directing groups is developed. The oxidant-free reaction is applicable to a wide range of heteroarene substrates, including 2-pyridones, indoles, aryl rings, pyrroles and carbazoles. It allows installation of CD groups under straightforward reaction conditions.
View Article and Find Full Text PDFA one-pot strategy with yields up to 82% was reported to generate 2-(pyridin-2-yl)-2-(3,3a,6-tris(5-pyridin-2-yl)-5-oxohexahydropyrrolo[3,2-] pyrrol-2(1)-ylidene)acetonitrile and its derivatives -. Silica gel promoted quantitative conversion from stable intermediate to within 30 min at room temperature. Finally, four chemical σ bonds and two chiral carbons with high diastereoselectivity were achieved.
View Article and Find Full Text PDFThe obscure theory of passive subambient daytime radiative cooling (PSDRC) was deduced in a more understandable way using an arithmetic formula rather than integro-differential equations. Based on two boundary conditions of the equations, an innovative radiative cooler was successfully developed to qualitatively observe PSDRC phenomena and quantitatively characterize the cooling effect and cooling power of radiative cooling coatings (RC coatings). The remarkable subambient temperature reduction over 4.
View Article and Find Full Text PDFThe first Rh -catalyzed, directed decarbonylative C2-H alkenylation of imidazoles with readily available alkenyl carboxylic acids is reported. The reaction proceeds in a highly regio- and stereoselective manner, providing efficient access to C2-alkenylated imidazoles that are generally inaccessible by known C-H alkenylation methods. This transformation accommodates a wide range of alkenyl carboxylic acids, including challenging conjugated polyene carboxylic acids, and diversely decorated imidazoles with high functional group compatibility.
View Article and Find Full Text PDFBackground: Coronary artery distension and aneurysm are complications of Kawasaki disease in children.
Purpose: To develop a Z-score regression model for coronary artery diameter in children that could be used as reference.
Material And Methods: This retrospective analysis included children with normal heart structure between March 2013 and April 2017.
Proc Natl Acad Sci U S A
November 2021
We report a molecular switching ensemble whose states may be regulated in synergistic fashion by both protonation and photoirradiation. This allows hierarchical control in both a kinetic and thermodynamic sense. These pseudorotaxane-based molecular devices exploit the so-called Texas-sized molecular box (cyclo[2]-(2,6-di(1H-imidazol-1-yl)pyridine)[2](1,4-dimethylenebenzene); 1, studied as its tetrakis-PF salt) as the wheel component.
View Article and Find Full Text PDFA highly selective palladium-catalyzed carbonylative arylation of weakly acidic benzylic C(sp)-H bonds of azaarylmethylamines with aryl bromides under 1 atm of CO gas has been achieved. This work represents the first examples of use of such weakly acidic pronucleophiles in this class of transformations. In the presence of a NIXANTPHOS-based palladium catalyst, this one-pot cascade process allows a range of azaarylmethylamines containing pyridyl, quinolinyl and pyrimidyl moieties and acyclic and cyclic amines to undergo efficient reactions with aryl bromides and CO to provide α-amino aryl-azaarylmethyl ketones in moderate to high yields with a broad substrate scope and good tolerance of functional groups.
View Article and Find Full Text PDFCo(III)-catalyzed highly regio- and stereoselective direct C6 olefination of 2-pyridones with alkynes has been developed with the assistance of chelation. Upon variation of the reaction conditions, 2-pyridones react well with diaryl alkynes via a C6 olefination/directing group migration pathway to give the tetrasubstituted 6-vinyl-2-pyridones, but the C6-H olefination with terminal alkynes works effectively to afford only the C6-olefinated 2-pyridones. A judicious choice of a solvent and an additive is crucial for catalysis.
View Article and Find Full Text PDFCp*Rh(III)-catalyzed chelation-assisted direct C-H bond functionalization of 1-(2-pyridyl)-2-pyridones with internal alkynes that can be controlled to give three different products in good yields has been realized. Depending on the reaction conditions, solvents and additives, the reaction pathway can be switched between alkenylation, alkenylation/directing group migration and rollover annulation. These reaction manifolds allow divergent access to a variety of valuable C6-alkenylated 1-(2-pyridyl)-2-pyridones, (Z)-6-(1,2-diaryl-2-(pyridin-2-yl)vinyl)pyridin-2(1H)-ones and 10H-pyrido[1,2-a][1,8]naphthyridin-10-ones from the same starting materials.
View Article and Find Full Text PDFAxisymmetric extension of beam steering angles by metasurfaces is of great interest due to its potential application in extending the angular scan range of existing phased arrays. This angle-multiplexed manipulation functionality requires anti-symmetrically angle-dispersive phase gradient, as well as anti-symmetric angular phase dispersion over continuous incident angles, which is difficult to be implemented by existing metasurfaces. In this work, a series of meta-atoms with asymmetric structures are developed to achieve the required phase response.
View Article and Find Full Text PDFThree-substituted 4-quinolizin-4-ones were obtained via a facile method with good selectivity and high efficiency. On the basis of alkyne substrate control, the mild and cost-efficient reaction has a broad substrate scope (20 examples, up to 93% yield) and is also easy to scale up. Active sites on the products allow for further modifications.
View Article and Find Full Text PDFSubambient daytime radiative cooling (SDRC) provides a promising electricity- and cryogen-free pathway for global energy-efficiency. However, current SDRC systems require stringent surface designs, which are neither cost-effective nor eco-friendly, to selectively emit thermal radiation to outer space and simultaneously maximize solar reflectance. Here, a generic method is developed to upgrade the conventional building-coating materials with a peculiar self-adaptive SDRC effect through combining particle scattering, sunlight-excited fluorescence, and mid-infrared broadband radiation.
View Article and Find Full Text PDFA Rh-catalyzed chelation-assisted C6-selective C-H activation/alkylation of 2-pyridones with readily available alkyl carboxylic acids or anhydrides is introduced. The reaction proceeds via substrate decarbonylation. This approach merges C-H functionalization with readily available anhydrides, allowing for the efficient synthesis of various C6-alkylated 2-pyridones with good functional group tolerance.
View Article and Find Full Text PDFA versatile Rh(i)-catalyzed C6-selective decarbonylative C-H alkenylation of 2-pyridones with readily available, and inexpensive alkenyl carboxylic acids has been developed. This directed dehydrogenative cross-coupling reaction affords 6-alkenylated 2-pyridones that would otherwise be difficult to access using conventional C-H functionalization protocols. The reaction occurs with high efficiency and is tolerant of a broad range of functional groups.
View Article and Find Full Text PDFThe first thermally stable and pH-responsive quadruplex intercalated motif (i-motif) structure formed by l-DNA is presented. Although this l-type i-motif exhibits the same physiochemical properties as its d isomer, its inverted chirality and good enzymatic resistance potentially open the way to the development of new DNA materials of pharmaceutical and biological interest.
View Article and Find Full Text PDFIsobutanol serves as an ideal gasoline additive owing to its good compatibility with current engine technology, high energy density, and high octane number. Herein, an efficient and selective Mn-catalyzed upgrading of ethanol with methanol into isobutanol is reported. This is the first example of deoxygenative coupling of lower alcohols to isobutanol by using a homogeneous non-noble-metal catalyst.
View Article and Find Full Text PDFThis study reports the first experimental evidence of DNA origami as a seed resulting in the increase in probability of protein crystallization. Using the DNA origami constructed from long single-stranded M13 DNA scaffolds folded with short single-stranded DNA staples, it was found that the addition of the DNA origami in concentrations of 2-6 nM to mixtures of a well-characterized protein (catalase) solution (1.0-7.
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