The field of analyte detection has benefitted greatly from the advent of colorimetric and fluorescent sensor arrays, which can uniquely sense analytes based on differential signals from indicator displacement events. Typically, several synthetic receptors that bind differentially to the analytes of interest must be developed through rational design and multistep syntheses. While the process of receptor development has been streamlined more recently by using dynamic combinatorial chemistry (DCC), the synthesis and isolation of individual receptors is still challenging and time-consuming, making sensor array development a laborious process. We developed a new approach to generating sensor arrays, termed “imprint-and-report,” that uses an entire dynamic combinatorial library (DCL) as each sensor in the array, such that isolating individual receptors is not necessary. The DCLs can be templated, or imprinted, with the analytes, followed by addition of a reporter fluorophore to facilitate indicator displacement interactions and subsequent analysis. This strategy is also successful when the DCLs are imprinted with the reporter and then each analyte is separately added before analysis. We have demonstrated the utility of this system for uniquely sensing all methylation states of Arg and Lys, as well as a set of dietary metabolites in human plasma samples with different levels of the metabolite biomarker. This DCL-based sensing system offers a high throughput approach to developing sensor arrays while also leveraging more of the chemical information stored within interacting noncovalent networks.

Development of “imprint-and-report” dynamic combinatorial sensor arrays: Applications to post-translational modifications (PTMs) and dietary metabolites

ACS Spring 2022

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