Gutenberg Open Science

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  • Item type:Item, ZeitschriftenaufsatzAccess status: Open Access ,
    Lipids and lipid nanoparticles functionalized with randomized poly(ethylene glycol) (rPEG) for mRNA delivery
    (2026)
    Dreier, Philip
    ;
    Bockhard, Caroline
    ;
    Seibel, David
    ;
    Soltwedel, Olaf
    ;
    Matthes, Rebecca
    PEG lipids are essential excipients in lipid nanoparticle (LNP) formulations and enable the transport of therapeutic ribonucleic acids, creating stealth properties for these nanocarriers. However, an increasing number of studies raise concerns related to the growing presence of anti-PEG antibodies (APA) in the population. The presence of APAs results in the recognition and accelerated blood clearance of PEGylated therapeutics, thus diminishing the desired stealth effect of PEGylation. In this study, we present the isomerization of PEG to randomized PEG (rPEG) as an efficient approach for inhibiting APA interaction while preserving the advantages of PEG. rPEGs were obtained via living anionic ring-opening (co)polymerization (AROP) of ethylene oxide (EO) with glycidyl methyl ether (GME). This yields rPEGs with narrow molar mass distributions (Mw/Mn = 1.04–1.10) for all EO:GME compositions synthesized. Chain-end functionalization of rPEGs with lipid anchor groups was conducted to obtain rPEG lipids with C14-chains (ditetradecylacetamide (DTAA), dimyristoyl-glycerol (DMG)). APA interaction was investigated via enzyme-linked immunosorbent assay (ELISA) and X-ray reflectometry (XRR) at monolayers of the rPEG lipid, allowing for a general understanding of the relation between the chain architecture and APA interaction. LNPs containing rPEG lipids were formulated and compared to established PEG-based LNPs, showing similar particle sizes, encapsulation and transfection efficiencies, and cell viabilities for a variety of cell lines. It is demonstrated that rPEG lipids can prevent APA binding but nevertheless exhibit similar performance in LNPs as comparable PEG lipids.
  • Item type:Item, ZeitschriftenaufsatzAccess status: Open Access ,
    Covalently linked ferrocene–polyoxometalate dyads for light-induced radical generation
    (2026)
    Knoll, Sebastian
    ;
    Schmidt, Heiner
    ;
    Sowa, Kevin
    ;
    Dietzek-Ivanšić, Benjamin
    ;
    Titze, Celina
    The design of covalently linked photoactive donor–acceptor dyads offers major opportunities for photocatalysis and solar energy conversion. Here, we report a noble metal-free dyad obtained by covalent anchoring of a ferrocene moiety to a Dawson-type polyoxotungstate. The resulting dyad shows visible light photoinduced charge-separation and electron transfer from the ferrocene to the polyoxometalate. The separated charges can be used for the photoinduced, oxidative and reductive activation of organic peroxides to generate oxygen-based radicals. Structural and mechanistic studies using in situ spectroscopy, time-resolved spectroscopy and spectro-electrochemistry as well as quantum chemical calculations shed light on the underlying photoinduced reactivity. The study presents a blueprint for the design of photoactive covalent photosensitizer–polyoxometalate dyads based on earth-abundant elements.
  • Item type:Item, DissertationAccess status: Open Access ,