Article
Polymer Science
David Siefker, Brandon A. Chan, Meng Zhang, Ju-Woo Nho, Donghui Zhang
Summary: This study demonstrates the zwitterionic ring-opening polymerization (ZROP) of sarcosine-derived N-thiocarboxyanhydrides (Me-NNTAs) using 1,1,3,3-tetramethylguanidine (TMG) initiators, resulting in well-defined polysarcosine polymers with controlled molecular weights and narrow molecular weight distributions. The polymerization exhibits living characteristics and can be conducted in the presence of moisture.
Article
Chemistry, Physical
Sarah Alamdari, Jim Pfaendtner
Summary: This study investigates the influence of the stereochemical properties of amino acid side chains on the folding structures of polypeptide chains. The results show that Nspe side chains tend to form left-handed helices, while Nrpe side chains tend to form right-handed helices. Additionally, it is found that the chemical properties of other side chains also affect the folding structures of polypeptide chains.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Polymer Science
Jingcheng Zou, Min Zhou, Zhemin Ji, Ximian Xiao, Yueming Wu, Ruxin Cui, Shuai Deng, Runhui Liu
Summary: This study presents a novel method for the synthesis of peptide/peptoid hybrid polymers with alternating distribution of residues, controlled molecular weight, and narrow dispersity. This method allows for quick synthesis of peptide mimicking peptide/peptoid hybrid polymers with adjustable proteolysis and opens up new possibilities for preparing novel peptide mimics with tunable proteolysis and large structural diversity.
Article
Chemistry, Multidisciplinary
Rachel E. Detwiler, Austin E. Schlirf, Jessica R. Kramer
Summary: Researchers have developed facile and high-yielding methods for preparing Pro and trans-4-acetoxy-Pro N-carboxyanhdrides (NCAs), and discovered a new initiator catalytic mechanism, opening up new avenues for synthesizing end-functional PP-based polypeptides with specific properties.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Polymer Science
Sofia L. Goodrich, Megan R. Hill, Rebecca A. Olson, Brent S. Sumerlin
Summary: The use of NPPOC as a photoprotecting group for primary amine initiators in NCAs polymerizations showed better polymerization control than previous methods. The addition of a small equivalence of base enhanced the control and resulted in polymers with lower dispersities. This method advances photo-controlled polypeptide synthesis by demonstrating high chain-end fidelity, efficient chain extension, and the ability to synthesize block copolymers.
Article
Polymer Science
Qingda Yan, Xue Dong, Rongze Xie, Xiufang Xu, Xiaoyan Wang, Ke Zhang, Jingya Xia, Jun Ling, Fei Zhou, Jihong Sun
Summary: Magnetic resonance imaging (MRI) is widely used in clinical diagnosis, with poly(alpha-amino acid)s being excellent carriers for MRI contrast agents. Mn2+@DoS micelles exhibit high longitudinal relaxivity and effective MRI contrast enhancement, showing great potential for clinical application as a novel MRI contrast agent.
JOURNAL OF MACROMOLECULAR SCIENCE PART A-PURE AND APPLIED CHEMISTRY
(2021)
Article
Polymer Science
Bailee N. Barrett, Garrett L. Sternhagen, Donghui Zhang
Summary: In this study, a well-controlled polymerization of poly(N-(3-tert-butoxy-3-oxopropyl) glycine) was achieved, producing polymers with narrow molecular weight distribution. The cloaked carboxyl groups on the polymer can be easily revealed under mild acidic conditions to yield a structural mimic of poly(glutamic acid), poly(N-(2-carboxyethyl) glycine, whose hydrodynamic size can be controlled by solution pH.
Article
Biochemistry & Molecular Biology
Botuo Zheng, Songyi Xu, Xufeng Ni, Jun Ling
Summary: This study achieved controlled NNTA polymerization in amide polar solvents by adding acetic acid as a promoter, producing polypeptoids with designable molecular weights and low dispersities. The presence of acetic acid not only accelerated polymerization, but also suppressed H2S-catalyzed decomposition, leading to preparation of high molecular weight polysarcosines.
Article
Polymer Science
Leon Capeloa, David Schwiertz, Matthias Barz
Summary: In this study, a method for the synthesis of multi-segment star polymers based on polypept(o)ides was reported. By introducing a multifunctional lysine end group and using living ring-opening polymerization (ROP), polymeric arms of different chemical nature could be synthesized separately. The successful and controlled synthesis of asymmetric miktoarm star polymers with precise control over the degree of polymerization was confirmed by 1H NMR and SEC experiments.
EUROPEAN POLYMER JOURNAL
(2023)
Article
Polymer Science
Pedro Salas-Ambrosio, Antoine Tronnet, Mostafa Badreldin, Sifan Ji, Sebastien Lecommandoux, Simon Harrisson, Pierre Verhaeghe, Colin Bonduelle
Summary: This report provides a comprehensive study on the contribution of the N-alkyl group to the synthesis of NNCA and its reactivity in polymerization reactions. We found that electron-donating groups can enhance the kinetic rates of polymerization reactions.
Article
Polymer Science
Shuo Wang, Hua Lu
Summary: This study reports a method for synthesizing thiol-functionalized polypeptides, which successfully suppresses the intramolecular isomerization side reactions and achieves homo-and copolypeptides with improved yield, high molecular weight, and narrow molecular weight distributions by selecting appropriate reaction solvents and adding benzoic acid as an additive. In addition, successful postpolymerization modifications of the D-Pen-containing copolypeptides on the tertiary thiols are achieved with high efficiency through thiol-Michael, SN2, and nitrosylation reactions. This work provides an efficient protection-free approach to generating functional polypeptides and creates a fundamental understanding for Pen-NCA chemistry.
Article
Multidisciplinary Sciences
Yali Hu, Zi-You Tian, Wei Xiong, Dedao Wang, Ruichi Zhao, Yan Xie, Yu-Qin Song, Jun Zhu, Hua Lu
Summary: This study presents a water-assisted controlled ring-opening polymerization method for ProNCA, which enables the rapid synthesis of well-defined PLP in a short time. The use of water facilitates proton shift and lowers the energy barrier, leading to fast and efficient reactions. The protein-mediated ROP of ProNCA offers a convenient approach for the synthesis of various protein-PLP conjugates with enhanced properties.
NATIONAL SCIENCE REVIEW
(2022)
Article
Materials Science, Biomaterials
Tobias Alexander Bauer, Jonas Eckrich, Nadine Wiesmann, Felix Kuczelinis, Wen Sun, Xiaolong Zeng, Benjamin Weber, Si Wu, Nicolas Hubert Bings, Sebastian Strieth, Matthias Barz
Summary: The study demonstrates the combination of light-sensitive polypyridyl-ruthenium(ii) complexes with polypept(o)ides to form photocleavable core cross-linked polymeric micelles, which have the potential for drug release and enhanced stability. Analysis shows increased cytotoxicity with micellar delivery of [Ru(bpy)(2)(H2O)(2)](2+) and mostly irradiation damage for [Ru(biq)(2)(H2O)(2)](2+), pointing towards the future development of quick-release complexes with stable circulation.
JOURNAL OF MATERIALS CHEMISTRY B
(2021)
Article
Pharmacology & Pharmacy
Christoph Wilhelmy, Isabell Sofia Keil, Lukas Uebbing, Martin A. Schroer, Daniel Franke, Thomas Nawroth, Matthias Barz, Ugur Sahin, Heinrich Haas, Mustafa Diken, Peter Langguth
Summary: Lipid nanoparticles (LNPs) have shown potential as carriers for mRNA-based therapeutics, however, their structure and efficacy are not fully understood. In this study, different lipid combinations were compared, and it was found that LNPs containing polysarcosine as stealth moieties showed improved activity and higher transfection efficiency. The use of small-angle X-ray scattering (SAXS) provided valuable information for the rational development of LNPs.
Review
Pharmacology & Pharmacy
Yong Liu, Lichen Yin
Summary: Gene therapy has gained significant attention for disease prevention and treatment. Polypeptides are commonly used for nucleic acid delivery due to their versatility and low cytotoxicity, with chemistry playing a crucial role in developing innovative polypeptides for efficient gene vectors. Recent chemical advances in polypeptide-based nucleic acid delivery vehicles have shown promise in overcoming extracellular and intracellular barriers, enabling successful gene transfection in vitro and in vivo.
ADVANCED DRUG DELIVERY REVIEWS
(2021)
Article
Materials Science, Multidisciplinary
Chen Hu, Lukas Hahn, Mengshi Yang, Alexander Altmann, Philipp Stahlhut, Juergen Groll, Robert Luxenhofer
Summary: This study presents a hybrid system of nanoclay and thermoresponsive block copolymer as a novel biomaterial ink, demonstrating improved mechanical properties and enhanced printing quality for extrusion-based bioprinting.
JOURNAL OF MATERIALS SCIENCE
(2021)
Article
Chemistry, Physical
Sebastian Endres, Emil Karaev, Simon Hanio, Jonas Schlauersbach, Christian Kraft, Tim Rasmussen, Robert Luxenhofer, Bettina Boettcher, Lorenz Meinel, Ann-Christin Poeppler
Summary: The study revealed that PF127 interferes with bile in simulated intestinal fluid, while pOx/pOzi is classified as non-interfering. When EFV is involved, PF127/EFV formulations exhibit concentration-dependent aggregation in the intestinal fluid, forming different types of colloids, while pOx/pOzi/EFV formulations form joint aggregates across the concentration range.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Polymer Science
Solomiia Borova, Christine Schlutt, Joachim Nickel, Robert Luxenhofer
Summary: This study introduces a postpolymerization modification method for polysarcosine, which allows for straightforward modification with nucleophiles. The method yields polymers with well-defined molar mass and high end-group fidelity, making it of interest for bioconjugation. However, further optimization is needed, especially for protein conjugation.
MACROMOLECULAR CHEMISTRY AND PHYSICS
(2022)
Article
Polymer Science
Qing Yu, Richard M. England, Anders Gunnarsson, Robert Luxenhofer, Kevin Treacher, Marianne B. Ashford
Summary: Polymeric micelles have been widely utilized as nanocarriers for delivering chemotherapeutic agents to improve cancer treatment efficacy. Developing telodendrimer micelles as a nanocarrier for poorly water-soluble drugs, such as fulvestrant, has shown great promise in achieving high drug loading capacity and stability. The versatility of these telodendrimer-based micelle systems in efficiently delivering both conjugated and encapsulated drugs with high stability makes them a promising drug delivery system for various therapeutic targets.
Article
Nanoscience & Nanotechnology
Salvatore E. Drago, Emanuela F. Craparo, Robert Luxenhofer, Gennara Cavallaro
Summary: Two amphiphilic graft copolymers were synthesized in this study and used to prepare nanoparticles delivering Zileuton. The nanoparticles were encapsulated in water-soluble microparticles by spray-drying to overcome size limitations for inhalation therapy, achieving optimal lung deposition. This approach allowed for the release of 70% of the drug payload in 24 hours, indicating potential for efficient drug delivery.
NANOMEDICINE-NANOTECHNOLOGY BIOLOGY AND MEDICINE
(2021)
Article
Engineering, Biomedical
Chen Hu, Taufiq Ahmad, Malik Salman Haider, Lukas Hahn, Philipp Stahlhut, Juergen Groll, Robert Luxenhofer
Summary: An advanced hybrid hydrogel ink was developed to improve the challenges in 3D printing with alginate bioink, and showed high shape fidelity and excellent stackability. Cell-laden printing and culture demonstrated good cytocompatibility and feasibility.
Article
Chemistry, Multidisciplinary
Matthias Beudert, Lukas Hahn, Anselm H. C. Horn, Niklas Hauptstein, Heinrich Sticht, Lorenz Meinel, Robert Luxenhofer, Marcus Gutmann
Summary: This study demonstrates the use of 3D printing technology to spatially control drug incorporation in biomaterials. By linking the release of a biologic (IGF-I) to matrix metalloproteinases (MMP), researchers have successfully developed a copolymer hydrogel that can release the bioactive drug in response to specific enzymes. The hydrogel system was further utilized for shape control and localized drug incorporation using extrusion 3D printing.
JOURNAL OF CONTROLLED RELEASE
(2022)
Article
Polymer Science
Mengshi Yang, Malik Salman Haider, Stefan Forster, Chen Hu, Robert Luxenhofer
Summary: This study investigates polymer micelles based on poly(2-oxazoline) for the formulation of chiral and achiral drugs. It is found that the maximum drug loading is mainly determined by the structure of the hydrophobic repeat units, with little effect from chirality in the case of curcumin and paclitaxel. However, for chiral and racemic ibuprofen, the maximum drug loading is not affected by the polymer structure or chirality.
Article
Biochemistry & Molecular Biology
Malik Salman Haider, Arun Kumar Mahato, Anastasiia Kotliarova, Stefan Forster, Bettina Boettcher, Philipp Stahlhut, Yulia Sidorova, Robert Luxenhofer
Summary: A novel BT44 micellar nanoformulation based on POx with ultrahigh drug-loading capacity has been developed, showing improved absorption and blood-brain barrier penetration for potential treatment of neurodegenerative disorders. The formulation retained biological activity in cells and exhibited no acute toxic effects in mice, paving the way for further preclinical and clinical development.
Article
Materials Science, Multidisciplinary
Juliane C. Kade, Ezgi Bakirci, Biranche Tandon, Danila Gorgol, Miroslav Mrlik, Robert Luxenhofer, Paul D. Dalton
Summary: In this study, melt electrowriting was used for the first time to process a magnetic polymer-based blend. The presence of CI particles resulted in well-defined, highly porous structures or scaffolds. This technique showed potential for stimuli-responsive applications, such as 4D printing, with good cell viability and magnetic displacement capabilities.
MACROMOLECULAR MATERIALS AND ENGINEERING
(2022)
Article
Materials Science, Multidisciplinary
Larissa Kessler, Zeynab Mirzaei, Juliane C. Kade, Robert Luxenhofer
Summary: This study introduces melt electrowriting (MEW) as a processing method to obtain rapid-dissolving drug-releasing scaffolds, containing IND as a model drug, for sublingual drug delivery applications. The results show completely amorphous dispersion of the polymer and drug after MEW processing resulting in smooth and uniform fibers and rapid dissolution of the drug loaded scaffold.
ACS APPLIED POLYMER MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Lukas Hahn, Theresa Zorn, Josef Kehrein, Tobias Kielholz, Anna-Lena Ziegler, Stefan Forster, Benedikt Sochor, Ekaterina S. Lisitsyna, Nikita A. Durandin, Timo Laaksonen, Vladimir Aseyev, Christoph Sotriffer, Kay Saalwaechter, Maike Windbergs, Ann-Christin Poeppler, Robert Luxenhofer
Summary: This study describes a non-H-bonding mechanism for cooling-induced hydrogel formation in polymer self-assemblies. The interaction between hydrophilic and hydrophobic blocks affects the micelle packing parameter, leading to a transition from spherical micelles to worm-like micelles and ultimately inverse thermogelation. This mechanism could be relevant for other polymeric materials and their interaction in biological environments, with potential applications in drug delivery or biofabrication.
Article
Chemistry, Organic
Solomiia Borova, Robert Luxenhofer
Summary: In the past decade, poly(2-oxazoline)s have been widely studied as potential materials for various biomedical applications, such as drug delivery systems and tissue engineering. However, the synthesis of these polymers often involves problematic organic solvents. In this study, we investigated the use of a green solvent called dihydrolevoglucosenone (DLG) for the cationic ring-opening polymerization of 2-ethyl-2-oxazoline and 2-butyl-2-oxazoline. Our findings reveal that the chosen solvent is not inert under typical polymerization conditions, leading to side products and limited control over the polymerization process.
BEILSTEIN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Lukas Hahn, Theresa Zorn, Josef Kehrein, Tobias Kielholz, Anna-Lena Ziegler, Stefan Forster, Benedikt Sochor, Ekaterina S. Lisitsyna, Nikita A. Durandin, Timo Laaksonen, Vladimir Aseyev, Christoph Sotriffer, Kay Saalwaechter, Maike Windbergs, Ann-Christin Poeppler, Robert Luxenhofer
Summary: A non-H-bonding mechanism for cooling-induced reversible order-order transition and thermogelation of polymer self-assemblies was investigated. The interaction between hydrophilic and hydrophobic blocks affects the micelle packing, resulting in the transition from spherical micelles to worm-like micelles and inverse thermogelation. The interaction pattern could be relevant for other polymeric materials and their interactions in biological environments, and controlling gel characteristics has potential applications in drug delivery or biofabrication.
Article
Polymer Science
Sebastian Halupczok, Maria Pfister, Annemarie Ringhand, Corinna Fetsch, Alevtina Cubukova, Antje Appelt-Menzel, Robert Luxenhofer
Summary: The partial reduction of poly(2-ethyl-2-oxazoline) was investigated, and a series of polymers were synthesized using different reduction methods. The reduction degree can be controlled by reaction time or stoichiometry, impacting the materials properties significantly.