Featured publications:
Surface Modification of Polyesters Using Biosourced Soil-Release Polymers
K. M. Starck, E. F. Fiandra, J. Binks, G. Si, R. Chilton, M. Sivik, R. L. Thompson, J. Li, M. R. Wilson and C. S. Mahon*
JACS Au, 2025, DOI: 10.1021/jacsau.4c00908
Soil-release polymers (SRPs) are important components of fabric care formulations, performing important roles in the cleaning of synthetic fabrics. SRPs modify the surface of textiles and render materials resistant to staining, while offering environmental benefits by enabling effective cleaning using shorter, cooler wash cycles. Most SRPs used in formulations contain petroleum-sourced terephthalic acid, limiting the environmental benefits presented by the use of these key additives. Here, we have prepared SRPs using a selection of pyridine dicarboxylate monomers that can be accessed from biomass and assessed their ability to modify polyester surfaces. Interestingly, a wide range of surface deposition behavior was observed, with soil-release performance significantly impacted by the pyridine dicarboxylate component in use. The performance of polymers containing 2,5-pyridine dicarboxylate units exceeded or was comparable to that of current industry-standard SRPs, while polymers constructed using 2,4- or 2,6-pyridine dicarboxylate units displayed poor performance. Through a range of studies including dynamic light scattering, contact angle analysis, scanning electron microscopy, and molecular modeling we have explored the solution and interfacial behavior of SRPs and propose the observed changes in performance to arise from a combination of differences in solution self-assembly and variation in affinities for polyester surfaces.
A glycopolymer sensor array that differentiates lectins and bacteria
K. G. Leslie, K. A. Jolliffe, M. Mullner, E. J. New, M. A. Fascione, W. B. Turnbull, V.-P. Friman and C. S. Mahon*
Biomacromolecules, 2024, 25, 7466-7474
Identification of bacterial lectins offers an attractive route to the development of new diagnostics, but the design of specific sensors is complicated by the low selectivity of carbohydrate−lectin interactions. Here we describe a glycopolymer-based sensor array which can identify a selection of lectins with similar carbohydrate recognition preferences through a pattern-based approach. Receptors were generated using a polymer scaffold functionalized with an environmentally sensitive fluorophore, along with simple carbohydrate motifs. Exposure to lectins induced changes in the emission profiles of the receptors, enabling the discrimination of analytes using linear discriminant analysis. The resultant algorithm was used for lectin identification across a range of concentrations and within complex mixtures of proteins. The sensor array was shown to discriminate different strains of pathogenic bacteria, demonstrating its potential application as a rapid diagnostic tool to characterize bacterial infections and identify bacterial virulence factors such as production of adhesins and antibiotic resistance.
Sugar-Coated: Can Multivalent Glycoconjugates Improve upon Nature’s Design?
K. G. Leslie, S. S. Berry, G. J. Miller* and C. S. Mahon*
J. Am. Chem. Soc., 2024, 146, 27215-27232
Multivalent interactions between receptors and glycans play an important role in many different biological processes, including pathogen infection, self-recognition, and the immune response. The growth in the number of tools and techniques towards the assembly of multivalent glycoconjugates means it is possible to create synthetic systems that more and more closely resemble the diversity and complexity we observe in nature. In this Perspective we give the background to the recognition and binding enabled by multivalent interactions in nature, and discuss the strategies used to construct synthetic glycoconjugate equivalents. We highlight key discoveries and the current state of the art in their applications to glycan arrays, vaccines, and other therapeutic and diagnostic tools, with an outlook towards some areas we believe are of most interest for future work in this area.
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:
M. Starck, E. F. Fiandra, J. Binks, G. Si, R. Chilton, M. Sivik, R. L. Thompson, J. Li, M. R. Wilson and C. S. Mahon,* Surface Modification of Polyesters Using Biosourced Soil-Release Polymers, JACS Au, 2025, DOI: 10.1021/jacsau.4c00908.
K. G. Leslie, K. A. Jolliffe, M. Mullner, E. J. New, M. A. Fascione, W. B. Turnbull, V.-P. Friman and C. S. Mahon,* A glycopolymer sensor array that differentiates lectins and bacteria. Biomacromolecules, 2024, 25, 7466-7474
K. G. Leslie, S. S. Berry, G. J. Miller* and C. S. Mahon,* Sugar-Coated: Can Multivalent Glycoconjugates Improve upon Nature’s Design? J. Am. Chem. Soc., 2024, 146, 27215-27232
H. S. Wootton, S. S. Berry, E. L. Ferguson, C. S. Mahon and G. J. Miller, * G. J., Adaptable Synthesis of Chondroitin Sulfate Disaccharide Subtypes Preprogrammed for Regiospecific O-Sulfation. Eur. J. Org. Chem., 2024, e202400587
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.