| 2020 |
Massi L, Najer A, Chapman R, Spicer CD, Nele V, Che J, et al., 'Tuneable peptide cross-linked nanogels for enzyme-triggered protein delivery', Journal of Materials Chemistry B, 8 8894-8907 (2020)
© The Royal Society of Chemistry 2020. Many diseases are associated with the dysregulated activity of enzymes, such as matrix metalloproteinases (MMPs). This dysregulation can be ... [more] © The Royal Society of Chemistry 2020. Many diseases are associated with the dysregulated activity of enzymes, such as matrix metalloproteinases (MMPs). This dysregulation can be leveraged in drug delivery to achieve disease- or site-specific cargo release. Self-assembled polymeric nanoparticles are versatile drug carrier materials due to the accessible diversity of polymer chemistry. However, efficient loading of sensitive cargo, such as proteins, and introducing functional enzyme-responsive behaviour remain challenging. Herein, peptide-crosslinked, temperature-sensitive nanogels for protein delivery were designed to respond to MMP-7, which is overexpressed in many pathologies including cancer and inflammatory diseases. The incorporation ofN-cyclopropylacrylamide (NCPAM) intoN-isopropylacrylamide (NIPAM)-based copolymers enabled us to tune the polymer lower critical solution temperature from 33 to 44 °C, allowing the encapsulation of protein cargo and nanogel-crosslinking at slightly elevated temperatures. This approach resulted in nanogels that were held together by MMP-sensitive peptides for enzyme-specific protein delivery. We employed a combination of cryogenic transmission electron microscopy (cryo-TEM), dynamic light scattering (DLS), small angle neutron scattering (SANS), and fluorescence correlation spectroscopy (FCS) to precisely decipher the morphology, self-assembly mechanism, enzyme-responsiveness, and model protein loading/release properties of our nanogel platform. Simple variation of the peptide linker sequence and combining multiple different crosslinkers will enable us to adjust our platform to target specific diseases in the future.
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| 2020 |
Wang Y, Cheng YT, Cao C, Oliver JD, Stenzel MH, Chapman R, 'Polyion Complex-Templated Synthesis of Cross-Linked Single-Enzyme Nanoparticles', MACROMOLECULES, 53 5487-5496 (2020)
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| 2020 |
Li Z, Ganda S, Melodia D, Boyer C, Chapman R, 'Well-Defined Polymers for Nonchemistry Laboratories using Oxygen Tolerant Controlled Radical Polymerization', JOURNAL OF CHEMICAL EDUCATION, 97 549-556 (2020)
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| 2020 |
Farazi S, Chen F, Foster H, Boquiren R, McAlpine SR, Chapman R, 'Real time monitoring of peptide delivery in vitro using high payload pH responsive nanogels', POLYMER CHEMISTRY, 11 425-432 (2020)
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| 2020 |
Li K, Chen F, Wang Y, Stenzel MH, Chapman R, 'Polyion Complex Micelles for Protein Delivery Benefit from Flexible Hydrophobic Spacers in the Binding Group', Macromolecular Rapid Communications, 41 (2020)
© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Although a range of polymer¿protein polyion complex (PIC) micelle systems have been developed in the literature, relatively... [more] © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Although a range of polymer¿protein polyion complex (PIC) micelle systems have been developed in the literature, relatively little attention has been paid to the influence of polymer structure on the assembly, or to the mechanism of disassembly. In this work, Förster resonance energy transfer is used in combination with light sheet fluorescence microscopy and isothermal calorimetry to monitor the formation and stability of PIC micelles with various carboxylic-acid-based binding blocks in MCF-7 cancer spheroid models. All micelles are stable in the presence of free protein, but are unstable in solutions with an ionic strength >200 mm and prone to disassembly at reduced pH. Introducing carbon spacers between the backbone and the binding carboxylic acid results in improved PIC micelle stability at physiological pH, but also increases the pKa of the binding moiety, resulting in improved protein release upon cell uptake. These results give important insights into how to tune PIC micelle stability for controlled protein release in biological environments.
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| 2020 |
Zheng P, Zhang X, Duan Y, Yan M, Chapman R, Jiang Y, Li H, 'Oxidation of graphene with variable defects: alternately symmetrical escape and self-restructuring of carbon rings', Nanoscale, 12 10140-10148 (2020)
Variable defects such as vacancies and grain boundaries are unavoidable in the synthesis of graphene, but play a central role in the activation of oxidation. Here, we apply reacti... [more] Variable defects such as vacancies and grain boundaries are unavoidable in the synthesis of graphene, but play a central role in the activation of oxidation. Here, we apply reactive molecular dynamics simulations to reveal the underpinning mechanisms of oxidation in graphene with or without defects at the atomic scale. There exist four oxidation modes generating CO2 or CO in different stages, beginning from a single-atom vacancy, and proceeding until the ordered structure broken down into carbon oxide chains. The oxidation process of the graphene sheets experiences four typical stages, in which alternately symmetrical escape phenomenon is observed. Importantly, disordered rings can self-restructure during the oxidation of grain boundaries. Of all defects, the oxidation of vacancy has the lowest energy barrier and is therefore the easiest point of nucleation. This study demonstrates the crucial role of defects in determining the oxidation kinetics, and provides theoretical guidance for the oxidation prevention of graphene and the production of functionalized graphene.
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| 2019 |
Chapman R, Stenzel MH, 'All Wrapped up: Stabilization of Enzymes within Single Enzyme Nanoparticles', JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 141 2754-2769 (2019)
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| 2019 |
Li Z, Kosuri S, Foster H, Cohen J, Jumeaux C, Stevens MM, et al., 'A Dual Wavelength Polymerization and Bioconjugation Strategy for High Throughput Synthesis of Multivalent Ligands', JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 141 19823-19830 (2019)
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| 2019 |
Oliver S, Zhao L, Gormley AJ, Chapman R, Boyer C, 'Living in the Fast Lane High Throughput Controlled/Living Radical Polymerization', MACROMOLECULES, 52 3-23 (2019)
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| 2019 |
Rahimi MN, Foster HG, Farazi SN, Chapman R, McAlpine SR, 'Polymer mediated transport of the Hsp90 inhibitor LB76, a polar cyclic peptide, produces an Hsp90 cellular phenotype', CHEMICAL COMMUNICATIONS, 55 4515-4518 (2019)
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| 2019 |
Chen F, Raveendran R, Cao C, Chapman R, Stenzel MH, 'Correlation between polymer architecture and polyion complex micelle stability with proteins in spheroid cancer models as seen by light- sheet microscopy', POLYMER CHEMISTRY, 10 1221-1230 (2019)
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| 2018 |
Gormley AJ, Yeow J, Ng G, Conway Ó, Boyer C, Chapman R, 'An Oxygen-Tolerant PET-RAFT Polymerization for Screening Structure-Activity Relationships', Angewandte Chemie, 130 1573-1578 (2018)
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| 2018 |
Yeow J, Joshi S, Chapman R, Boyer C, 'A Self-Reporting Photocatalyst for Online Fluorescence Monitoring of High Throughput RAFT Polymerization', Angewandte Chemie, 130 10259-10263 (2018)
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| 2018 |
Ishizuka F, Chapman R, Kuche RP, Coureault M, Zetterlund PB, Stenzel MH, 'Polymeric Nanocapsules for Enzyme Stabilization in Organic Solvents', MACROMOLECULES, 51 438-446 (2018)
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| 2018 |
Ng G, Yeow J, Chapman R, Isahak N, Wolyetang E, Cooper-White JJ, Boyer C, 'Pushing the Limits of High Throughput PET-RAFT Polymerization', MACROMOLECULES, 51 7600-7607 (2018)
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| 2018 |
Yeow J, Chapman R, Gormley AJ, Boyer C, 'Up in the air: oxygen tolerance in controlled/living radical polymerisation', CHEMICAL SOCIETY REVIEWS, 47 4357-4387 (2018)
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| 2018 |
Gormley AJ, Yeow J, Ng G, Conway O, Boyer C, Chapman R, 'An Oxygen-Tolerant PET-RAFT Polymerization for Screening Structure-Activity Relationships', ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 57 1557-1562 (2018)
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| 2018 |
Yeow J, Joshi S, Chapman R, Boyer C, 'A Self-Reporting Photocatalyst for Online Fluorescence Monitoring of High Throughput RAFT Polymerization', ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 57 10102-10106 (2018)
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| 2018 |
Milner PE, Parkes M, Puetzer JL, Chapman R, Stevens MM, Cann P, Jeffers JRT, 'A low friction, biphasic and boundary lubricating hydrogel for cartilage replacement', ACTA BIOMATERIALIA, 65 102-111 (2018)
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| 2017 |
Yeow J, Chapman R, Xu J, Boyer C, 'Oxygen tolerant photopolymerization for ultralow volumes', POLYMER CHEMISTRY, 8 5012-5022 (2017)
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| 2017 |
Chapman R, Melodia D, Qu J-B, Stenzel MH, 'Controlled poly(olefin)s via decarboxylation of poly(acrylic acid)', POLYMER CHEMISTRY, 8 6636-6643 (2017)
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| 2017 |
Qu J-B, Chapman R, Chen F, Lu H, Stenzel MH, 'Swollen Micelles for the Preparation of Gated, Squeezable, pH Responsive Drug Carriers', ACS APPLIED MATERIALS & INTERFACES, 9 13865-13874 (2017)
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| 2016 |
Chapman R, Gormley AJ, Stenzel MH, Stevens MM, 'Combinatorial Low-Volume Synthesis of Well-Defined Polymers by Enzyme Degassing', ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 55 4500-4503 (2016)
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| 2016 |
Liu NJ, Chapman R, Lin Y, Mmesi J, Bentham A, Tyreman M, et al., 'Point of care testing of phospholipase A2 group IIA for serological diagnosis of rheumatoid arthritis', NANOSCALE, 8 4482-4485 (2016)
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| 2016 |
Liu NJ, Chapman R, Lin Y, Bentham A, Tyreman M, Philips N, et al., 'Phospholipase A2 as a point of care alternative to serum amylase and pancreatic lipase', NANOSCALE, 8 11834-11839 (2016)
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| 2015 |
Lin Y, Chapman R, Stevens MM, 'Integrative Self-Assembly of Graphene Quantum Dots and Biopolymers into a Versatile Biosensing Toolkit', ADVANCED FUNCTIONAL MATERIALS, 25 3183-3192 (2015)
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| 2015 |
Harrison RH, Steele JAM, Chapman R, Gormley AJ, Chow LW, Mahat MM, et al., 'Modular and Versatile Spatial Functionalization of Tissue Engineering Scaffolds through Fiber-Initiated Controlled Radical Polymerization', ADVANCED FUNCTIONAL MATERIALS, 25 5748-5757 (2015)
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| 2015 |
Jumeaux C, Chapman R, Chandrawati R, Stevens MM, 'Synthesis and self-assembly of temperature-responsive copolymers based on N-vinylpyrrolidone and triethylene glycol methacrylate', POLYMER CHEMISTRY, 6 4116-4122 (2015)
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| 2015 |
Chapman R, Lin Y, Burnapp M, Bentham A, Hillier D, Zabron A, et al., 'Multivalent Nanoparticle Networks Enable Point-of-Care Detection of Human Phospholipase-A2 in Serum', ACS NANO, 9 2565-2573 (2015)
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| 2014 |
Lin Y, Chapman R, Stevens MM, 'Label-Free Multimodal Protease Detection Based on Protein/Perylene Dye Coassembly and Enzyme-Triggered Disassembly', ANALYTICAL CHEMISTRY, 86 6410-6417 (2014)
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| 2014 |
Chapman R, Gormley AJ, Herpoldt K-L, Stevens MM, 'Highly Controlled Open Vessel RAFT Polymerizations by Enzyme Degassing', MACROMOLECULES, 47 8541-8547 (2014)
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| 2014 |
Blunden BM, Chapman R, Danial M, Lu H, Jolliffe KA, Perrier S, Stenzel MH, 'Drug Conjugation to Cyclic Peptide-Polymer Self-Assembling Nanotubes', CHEMISTRY-A EUROPEAN JOURNAL, 20 12745-12749 (2014)
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| 2014 |
Gormley AJ, Chapman R, Stevens MM, 'Polymerization Amplified Detection for Nanoparticle-Based Biosensing', NANO LETTERS, 14 6368-6373 (2014)
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| 2013 |
Chapman R, Jolliffe KA, Perrier S, 'Multi-shell Soft Nanotubes from Cyclic Peptide Templates', ADVANCED MATERIALS, 25 1170-1172 (2013)
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| 2013 |
Chapman R, Warr GG, Perrier S, Jolliffe KA, 'Water-Soluble and pH-Responsive Polymeric Nanotubes from Cyclic Peptide Templates', CHEMISTRY-A EUROPEAN JOURNAL, 19 1955-1961 (2013)
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| 2013 |
Chapman R, Bouten PJM, Hoogenboom R, Jolliffe KA, Perrier S, 'Thermoresponsive cyclic peptide - poly(2-ethyl-2-oxazoline) conjugate nanotubes', CHEMICAL COMMUNICATIONS, 49 6522-6524 (2013)
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| 2013 |
Chapman R, Koh ML, Warr GG, Jolliffe KA, Perrier S, 'Structure elucidation and control of cyclic peptide-derived nanotube assemblies in solution', CHEMICAL SCIENCE, 4 2581-2589 (2013)
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| 2012 |
Chapman R, Danial M, Koh ML, Jolliffe KA, Perrier S, 'Design and properties of functional nanotubes from the self-assembly of cyclic peptide templates', CHEMICAL SOCIETY REVIEWS, 41 6023-6041 (2012)
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| 2012 |
Wilkinson BL, Day S, Chapman R, Perrier S, Apostolopoulos V, Payne RJ, 'Synthesis and Immunological Evaluation of Self-Assembling and Self-Adjuvanting Tricomponent Glycopeptide Cancer-Vaccine Candidates', CHEMISTRY-A EUROPEAN JOURNAL, 18 16540-16548 (2012)
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| 2012 |
Junkers T, Delaittre G, Chapman R, Guenzler F, Chernikova E, Barner-Kowollik C, 'Thioketone-Mediated Polymerization with Dithiobenzoates: Proof for the Existence of Stable Radical Intermediates in RAFT Polymerization', MACROMOLECULAR RAPID COMMUNICATIONS, 33 984-990 (2012)
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| 2012 |
Poon CK, Chapman R, Jolliffe KA, Perrier S, 'Pushing the limits of copper mediated azide-alkyne cycloaddition (CuAAC) to conjugate polymeric chains to cyclic peptides', POLYMER CHEMISTRY, 3 1820-1826 (2012)
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| 2011 |
Dehn S, Chapman R, Jolliffe KA, Perrier S, 'Synthetic Strategies for the Design of Peptide/Polymer Conjugates', POLYMER REVIEWS, 51 214-234 (2011)
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| 2011 |
Chapman R, Jolliffe KA, Perrier S, 'Modular design for the controlled production of polymeric nanotubes from polymer/peptide conjugates', POLYMER CHEMISTRY, 2 1956-1963 (2011)
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| 2010 |
Chapman R, Jolliffe KA, Perrier S, 'Synthesis of Self-assembling Cyclic Peptide-polymer Conjugates using Click Chemistry', AUSTRALIAN JOURNAL OF CHEMISTRY, 63 1169-1172 (2010)
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