Featured publications:
Designing biodegradable alternatives to commodity polymers
E. F. Fiandra, L. Shaw, M. Starck, C. J. McGurk and C. S. Mahon*
Chem. Soc. Rev., 2023, 52, 8085-8105
The development and widespread adoption of commodity polymers changed societal landscapes on a global scale. Without the everyday materials used in packaging, textiles, construction and medicine, our lives would be unrecognisable. Through decades of use, however, the environmental impact of waste plastics has become grimly apparent, leading to sustained pressure from environmentalists, consumers and scientists to deliver replacement materials. The need to reduce the environmental impact of commodity polymers is beyond question, yet the reality of replacing these ubiquitous materials with sustainable alternatives is complex. In this tutorial review, we will explore the concepts of sustainable design and biodegradability, as applied to the design of synthetic polymers intended for use at scale. We will provide an overview of the potential biodegradation pathways available to polymers in different environments, and highlight the importance of considering these pathways when designing new materials. We will identify gaps in our collective understanding of the production, use and fate of biodegradable polymers: from identifying appropriate feedstock materials, to considering changes needed to production and recycling practices, and to improving our understanding of the environmental fate of the materials we produce. We will discuss the current standard methods for the determination of biodegradability, where lengthy experimental timescales often frustrate the development of new materials, and highlight the need to develop better tools and models to assess the degradation rate of polymers in different environments.
Macromolecular Optical Sensor Arrays
Linda Mitchell, Elizabeth J. New, and Clare S. Mahon*
ACS Appl. Polym. Mater., 2021, 3, 506-530.
Chemical sensors play an important role in our understanding of chemical and biological systems, providing sensitive and rapid detection of a variety of substrates. Array-based sensing approaches avoid the ongoing challenge of designing and synthesizing selective receptors for particular analytes, a labor-intensive process that can frustrate the development of sensors. Instead, cross-reactive sensor arrays utilize multiple sensing elements that interact uniquely with each analyte and produce a distinct pattern of responses, enabling identification. To date, there are a variety of strategies both to gain cross-reactivity and diversity of sensors required for array-based sensing and to broaden the scope of analytes for detection. Sensor arrays constructed using macromolecular components such as polymers and nanoparticles offer an attractive route to the discrimination of multiple similar analytes, particularly within the context of biological sensing, where recognition over large areas is often required. Here, we focus on macromolecular sensing arrays underpinned by optical detection methods, which can enable rapid, sensitive detection of a range of analytes. We discuss the current state-of-the art and explore the challenges to be overcome in translating exciting scientific advances to applications beyond the laboratory.
Glycomacromolecules: Addressing challenges in drug delivery and therapeutic development
Will Stuart-Walker and Clare S. Mahon*
Adv. Drug Deliv. Rev., 2021, 171, 77-93.
Carbohydrate-based materials offer exciting opportunities for drug delivery. They present readily available, biocompatible components for the construction of macromolecular systems which can be loaded with cargo, and can enable targeting of a payload to particular cell types through carbohydrate recognition events established in biological systems. These systems can additionally be engineered to respond to environmental stimuli, enabling triggered release of payload, to encompass multiple modes of therapeutic action, or to simultaneously fulfil a secondary function such as enabling imaging of target tissue. Here, we will explore the use of glycomacromolecules to deliver therapeutic benefits to address key health challenges, and suggest future directions for development of next-generation systems.
E. E. Antunez, C. S. Mahon, Z. Tong, N. H. Voelcker and M. Müllner
Biomacromolecules, 2021, 22, 441-453.
Waterborne diarrheal diseases such as travelers’ diarrhea and cholera remain a threat to public health in many countries. Rapid diagnosis of an infectious disease is critical in preventing the escalation of a disease outbreak into an epidemic. Many of the diagnostic tools for infectious diseases employed today are time-consuming and require specialized laboratory settings and trained personnel. There is hence a pressing need for fit-for-purpose point-of-care diagnostic tools with emphasis in sensitivity, specificity, portability, and low cost. We report work toward thermally reversible biosensors for detection of the carbohydrate-binding domain of the Escherichia coli heat-labile enterotoxin (LTB), a toxin produced by enterotoxigenic E. coli strains, which causes travelers’ diarrhea. The biosensing platform is a hybrid of two materials, combining the optical properties of porous silicon (pSi) interferometric transducers and a thermoresponsive multivalent glycopolymer, to enable recognition of LTB. Analytical performance of our biosensors allows us to detect, using a label-free format, sub-micromolar concentrations of LTB in solution as low as 0.135 μM. Furthermore, our platform shows a temperature-mediated “catch-and-release” behavior, an exciting feature with potential for selective protein capture, multiple readouts, and regeneration of the sensor over consecutive cycles of use.
Publications:
E. F. Fiandra, L. Shaw, M. Starck, C. J. McGurk and C. S. Mahon,* Designing biodegradable alternatives to commodity polymers, Chem. Soc. Rev., 2023, 52, 8085-8105.
P. Singla, S. Kaur, O. Jamieson, A. Dann, S. Garg, C. S. Mahon, R. D. Crapnell, C. E. Banks, I. Kaur and M. Peeters, Electrochemical and thermal detection of allergenic substance lysozyme with molecularly imprinted nanoparticles Anal. Bioanal. Chem., 2023, DOI: 10.1007/s00216-023-04638-2
C. C. Piras, C. S. Mahon, P. G. Genever and D. K. Smith, Shaping and Patterning Supramolecular Materials─Stem Cell-Compatible Dual-Network Hybrid Gels Loaded with Silver Nanoparticles, ACS Biomater. Sci. Eng, 2022, 8, 1829-1840.
J. Wilkinson, A Boxall…C. S. Mahon…et al, Pharmaceutical pollution of the world’s rivers, Proc. Natl Acad. Sci. USA, 2022, 119, e2113947119.
T. Keenan, R. J. Spears, S. Akkad, C. S. Mahon, N. E. Hatton, J. Walton, A. Noble, N. D. Yates, C. G. Baumann, A. Parkin, N. Signoret and M. A. Fascione, A Tale of Two Bioconjugations: pH Controlled Divergent Reactivity of Protein α-oxo-Aldehydes in Competing α-oxo-Mannich and Catalyst-Free Aldol Ligations, ACS Chem. Biol., 2021, 16, 2387-2400.
W. Stuart-Walker and C. S. Mahon,* Glycomacromolecules: Addressing challenges in drug delivery and therapeutic development, Adv. Drug Deliv. Rev., 2021, 171, 77-93.
L. Mitchell, E. J. New and C. S. Mahon,* Macromolecular Optical Sensor Arrays, ACS Appl. Polym. Mater., 2021, 3, 506-530.
E. E. Antunez, C. S. Mahon, Z. Tong, N. H. Voelcker and M. Müllner, A Regenerable Biosensing Platform for Bacterial Toxins, Biomacromolecules, 2021, 22, 441-453.
T. Pelras, C. S. Mahon, Nonappa, M. Müllner, One-dimensional polyzwitterionic nanoparticles via interpolyelectrolyte complexation on molecular polymer brush templates, Macromol. Rapid Commun, 2020, 2000401.
C. Piras, C. S. Mahon, D. K. Smith, Self‐assembled supramolecular hybrid hydrogel beads loaded with silver nanoparticles for antimicrobial application, Chem. Eur. J., 2020, 26, 8452-8457.
X. Chen, W. Jiang, A. Ahmed, C. S. Mahon, M. Müllner, B. Cao and T. Xia, Engineering Protective Polymer Coatings for Liver Microtissues, Chem. Res. Toxicol., 2019, 32, 49-56.
C. S. Mahon,* M. L. Huang,* Highlights from Faraday Discussion 301: Nanolithography of Biointerfaces, London, UK, July 3–5 2019, Chem. Commun., 2019, 55, 13631-13637.
C. S. Mahon,* G. C. Wildsmith, D. Haksar, E. de Poel, R. Pieters, J. M. Beekman, M. Webb and W. B. Turnbull,* A ‘catch-and-release’ receptor for the cholera toxin, Faraday Discuss., 2019, 219, 112-117.
T. Pelras, C. S. Mahon, Nonappa, O. Ikkala, A.H. Gröschel, M. Müllner, Polymer nanowires with highly precise internal morphology and topography, J. Am. Chem. Soc., 2018, 140, 12736-12740.
T. Pelras, C. S. Mahon, M. Müllner, Synthesis and applications of compartmentalised polymer brushes, Angew. Chem. Int. Ed., 2018, 57, 6982-6994.
C. S. Mahon, C. J. McGurk, S. M. D. Watson, M. A. Fascione, C. Sakonsinsiri, W. B. Turnbull and D. A. Fulton, Molecular recognition-mediated transformation of single-chain polymer nanoparticles into crosslinked polymer films, Angew. Chem. Int. Ed., 2017, 56, 12913-12918.
M. Khuphe, C. S. Mahon and P. D. Thornton, Glucose-bearing biodegradable poly(amino acid) and poly(amino acid)-poly(ester) conjugates for controlled payload release, Biomater. Sci., 2016, 4, 1792-1801.
C. S. Mahon, M. A. Fascione, C. Sakonsinsiri, T. E. McAllister, W. B. Turnbull and D. A. Fulton, Templating carbohydrate-functionalised polymer-scaffolded dynamic combinatorial libraries with lectins, Org. Biomol. Chem., 2015, 13, 2756-2761.
C. S. Mahon and D. A. Fulton, Mimicking nature with synthetic macromolecules capable of recognition, Nature Chem., 2014, 6, 665-672.
C. S. Mahon and D. A. Fulton, Templation-induced re-equilibration in polymer-scaffolded dynamic combinatorial libraries leads to enhancements in binding affinities, Chem. Sci., 2013, 4, 3661-3666.
C. S. Mahon, A. W. Jackson, B. S. Murray and D. A. Fulton, Investigating templating within Polymer-Scaffolded Dynamic Combinatorial Libraries, Polym. Chem., 2013, 4, 368-377.
D. E. Whitaker, C. S. Mahon and D. A. Fulton, Thermoresponsive dynamic covalent single-chain polymer nanoparticles reversibly transform into a hydrogel, Angew. Chem., Int. Ed., 2013, 52, 956-959.
C. S. Mahon, A. W. Jackson, B. S. Murray and D. A. Fulton, Templating a polymer-scaffolded dynamic combinatorial library, Chem. Commun., 2011, 47, 7209-7211.
B. S. Murray, A. W. Jackson, C. S. Mahon and D. A. Fulton, Reactive thermoresponsive copolymer scaffolds, Chem. Commun., 2010, 46, 8651-8653.