Abstract
We here provide detailed insight in self-assembled complex coacervate systems exploiting gold nanoparticles for cryoTEM contrast. Nanoparticle-containing dendrimicelles are formed from fifth-generation dendrimer-encapsulated nanoparticles (DENs) and dendrimer-stabilized nanoparticles (DSNs). The complex coacervate structures self-organize in biconcave thin water layers into size-sorted monolayer superstructures. The embedded nanoparticles are a straightforward tool to visualize dendrimicelles and determine the aggregation number and polydispersity. The superstructure shows extreme size-sorting patterns which, contrary to related systems with higher generation dendrimers, consists not only of dendrimicelles but also much bigger complex coacervate nanoassemblies, such as vesicles.
Highlights
The dendrimicelles arranged following the thickness of the thin, biconcave-shaped, ice film, related to the increased size-sorting to an increased dendrimicelle polydispersity caused by a decreased micelle stability, corroborating with previous work by Wang et al on carboxylic acid-terminated PAMAM dendrimers that showed a generation-dependent dendrimicelle stability[13]
We here present dendrimicelles formed from generation five-based PAMAM dendrimers at various charge stoichiometries, and analyze the formed complex coacervate superstructures using cryoTEM and Dynamic Light Scattering techniques
Following the strategy that we reported before[22], we mixed the AuDENs with an anionic–neutral block copolymer, consisting of a 64-subunit polymethacrylic acid and a 885-subunit polyethyleneoxide block, pMAA64pEO885
Summary
Jan Bart ten Hove[1,2], Matthias N. van Oosterom[2], FijsW. B. van Leeuwen1,2 & Aldrik H.Velders 1,2. By incorporating dendrimers into the micelles, the unique encapsulation property of dendrimers can be used to “load” complex coacervate core micelles, as we recently showed by combining block copolymers together with DENs21,22, forming well-defined dendrimicelles that carried ~20–30 nanoparticles/dendrimicelle depending on the generation used These nanoparticle-containing dendrimicelles self-organized into distinct disk-like monolayer superstructures inside ~0.1 μm thick biconcave ice films formed during cryoTEM sample preparation[21]. The nanoparticle-loaded dendrimicelles are a powerful tool to investigate the formed structures with cryoTEM, even for systems in which the subcomponents consist of mixtures of different populations of dendrimer-particles ratios like for the fifth generation PAMAM DENs. Besides well-defined dendrimicelles, nanostructures were observed that are too large to be complex coacervate core micelles, but more likely vesicles. Both the catalytic activity inside dendrimicelles as well as the formed vesicles are currently investigated
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