The design and synthesis of two-dimensional (2D) polymers is a challenging task, hitherto achieved in solution only through the aid of a solid surface "template" or preorganization of the building blocks in a 2D confined space. We present a novel approach for synthesizing free-standing, covalently bonded, single-monomer-thick 2D polymers in solution without any preorganization of building blocks on solid surfaces or interfaces by employing shape-directed covalent self-assembly of rigid, disk-shaped building blocks having laterally predisposed reactive groups on their periphery. We demonstrate our strategy through a thiol-ene "click" reaction between (allyloxy)12CB[6], a cucurbit[6]uril (CB[6]) derivative with 12 laterally predisposed reactive alkene groups, and 1,2-ethanedithiol to synthesize a robust and readily transferable 2D polymer. We can take advantage of the high binding affinity of fully protonated spermine (positive charges on both ends) to CB[6] to keep each individual polymer sheet separated from one another by electrostatic repulsion during synthesis, obtaining, for the first-time ever, a single-monomer-thick 2D polymer in solution. The arrangement of CB[6] repeating units in the resulting 2D polymer has been characterized using gold nanoparticle labeling and scanning transmission electron microscopy. Furthermore, we have confirmed the generality of our synthetic approach by applying it to different monomers to generate 2D polymers. Novel 2D polymers, such as our CB[6] derived polymer, may be useful in selective transport, controlled drug delivery, and chemical sensing and may even serve as well-defined 2D scaffolds for ordered functionalization and platforms for bottom-up 3D construction.
Developing a material that can combat antibiotic-resistant bacteria, a major global health threat, is an urgent requirement. To tackle this challenge, we synthesized a multifunctional subphthalocyanine (SubPc) polymer nanosphere that has the ability to target, label, and photoinactivate antibiotic-resistant bacteria in a single treatment with more than 99 % efficiency, even with a dose as low as 4.2 J cm(-2) and a loading concentration of 10 nM. The positively charged nanosphere shell composed of covalently linked SubPc units can increase the local concentration of photosensitizers at therapeutic sites. The nanosphere shows superior performance compared to corresponding monomers presumably because of their enhanced water dispersibility, higher efficiency of singlet-oxygen generation, and phototoxicity. In addition, this material is useful in fluorescence labeling of living cells and shows promise in photoacoustic imaging of bacteria in vivo.
A metal-organic framework (MOF), NH(2)-MIL-101(Al), which acts as a bifunctional, site-isolated Lewis acid-Brønsted base heterogeneous catalyst, catalyzes a tandem Meinwald rearrangement-Knoevenagel condensation reaction with remarkable substrate selectivity.
EDGE ARTICLEAndrew J. deMello, Joshua B. Edel et al. Rapid cell extraction in aqueous twophase microdroplet systems PERSPECTIVE Barry M. Trost et al. Catalytic asymmetric allylic alkylation employing heteroatom nucleophiles: a powerful method for C-X bond formation
Developing am aterial that can combat antibioticresistant bacteria, am ajor global health threat, is an urgent requirement. To tackle this challenge,w es ynthesized am ultifunctional subphthalocyanine (SubPc) polymer nanosphere that has the ability to target, label, and photoinactivate antibiotic-resistant bacteria in as ingle treatment with more than 99 %efficiency,even with adose as lowas4.2 Jcm À2 and al oading concentration of 10 nm.T he positively charged nanosphere shell composed of covalently linked SubPc units can increase the local concentration of photosensitizers at therapeutic sites.The nanosphere shows superior performance compared to corresponding monomers presumably because of their enhanced water dispersibility,higher efficiency of singletoxygen generation, and phototoxicity.Inaddition, this material is useful in fluorescence labeling of living cells and shows promise in photoacoustic imaging of bacteria in vivo.
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