Fluorescent and catalytically active single chain nanoparticle (SCNP) systems allow for the visualization and tracing of the catalyst's distribution in a reaction system. We herein report a synthetic strategy to such SCNPs, generated through a photoactivated reaction at visible light (λ max = 415 nm) irradiation. Notably, the compaction reaction generates a fluorescent entity via a pro-fluorescent precursor. A polymer backbone (M n = 21,000 g mol −1 and Đ = 1.3), carrying phosphine ligands for the coordination of catalytically active gold complexes and the photoreactive orthomethylbenzaldehyde units and complementary alkyne moieties, was constructed based on nitroxide-mediated polymerization. The synthetic protocol entails an intermediate protection sequence for the catalyst-carrying phosphine unit to enable the installation of the cross-linking entities. The successful compaction of the SCNPs is demonstrated by a reduction in the chain's hydrodynamic volume via size exclusion chromatography and diffusion-ordered NMR spectroscopy.
Herein, we present an approach that allows versatile combination of inkjet-printed electronics and stretchable substrates. For this, we created a hybrid platform made out of stretchable Ecoflex covalently bonded via silane monolayers to flexible PET islands interconnected by bridges. The islands served as platforms where conductive lines, capacitive sensors and electrochromic devices were fabricated by inkjet printing. The robustness of the approach is highlighted by the minor influence of strain on the conductivity of printed Ag electrodes, which changed the resistance only by 1.3 % at an applied strain of 50 %. Furthermore, we demonstrated capacitor sensors capable of responding to strain changing their capacitance from 0.2 pF to 1.6 pF. To further show the applicability of the approach for multilayer/multimaterial optoelectronic elements, we processed electrochromic devices capable of displaying information on the stretchable platform. Thus, we demonstrate how this digital and additive concept can be applied for the scalable integration of printed optoelectronic devices onto stretchable systems without relying on lithographic processes.
We introduce a class of single‐chain nanoparticles (SCNPs) that respond to visible light (λmax=415 nm) with complete unfolding from their compact structure into linear chain analogues. The initial folding is achieved by a simple esterification reaction of the polymer backbone constituted of acrylic acid and polyethylene glycol carrying monomer units, introducing bimane moieties, which allow for the photochemical unfolding, reversing the ester‐bond formation. The compaction and the light driven unfolding proceed cleanly and are readily followed by size exclusion chromatography (SEC) and diffusion ordered NMR spectroscopy (DOSY), monitoring the change in the hydrodynamic radius (RH). Importantly, the folding reaction and the light‐induced unfolding are reversible, supported by the high conversion of the photo cleavage. As the unfolding reaction occurs in aqueous systems, the system holds promise for controlling the unfolding of SCNPs in biological environments.
In der vorliegenden Arbeit stellen wir Einzelketten‐Nanopartikel (ENPs) vor, die sich mit sichtbarem Licht (λmax=415 nm) aus ihrem gefalteten Zustand vollständig zu dem entsprechenden linearen Ausgangspolymer entfalten lassen. Die ursprüngliche Faltung wird durch eine einfache Veresterungsreaktion des Polymerrückrats, bestehend aus Acrylsäure und Polyethylenglykol‐dekorierten Acrylateinheiten, erreicht. Die so eingeführten Bimaneinheiten ermöglichen eine photochemische Entfaltungsreaktion durch Esterspaltung. Die Faltung und das lichtinduzierte Entfalten läuft weitgehend ohne Nebenreaktionen ab und kann direkt mittels Größenausschlusschromatographie (GPC) sowie diffusionsgeordneter NMR‐Spektroskopie (DOSY) durch die Veränderung des hydrodynamischen Radius (RH) nachverfolgt werden. Besonders hervorzuheben ist die Reversibilität sowohl der Faltung als auch der lichtinduzierten Entfaltung, die durch den hohen Umsatz bei der photochemischen Esterspaltung erreicht werden kann. Da die Photolyse in wässrigem Medium abläuft, könnte sich das System für die Untersuchung der Entfaltung von ENPs im biologischen Kontext eignen.
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