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Polymer Size-Catalytic Activity Relationships in Solution by Fluorescence Correlation Spectroscopy #MMPMID41319180
Pham VHB; Blum SA
Chemistry 2025[Nov]; ? (?): e02589 PMID41319180show ga
Measuring the catalytic activity of specific sizes of polymers with active catalysts in solution is typically challenging, due to limited instrument detection sensitivity and/or dynamic range. Here, a fluorescence correlation spectroscopy (FCS) method is developed to determine the catalytic activity of living polymers of a specific apparent size in solution. Deviation from a single-component FCS data fitting, as assessed by chi(2), is also introduced and developed as a "speciation index"-a method to evaluate and track changes in the relative amount of distinct polymer sizes with reaction progress. These methods are enabled by incorporating a selectively reactive fluorescent monomer into growing polydicyclopentadiene or polynorbornene during ring-opening metathesis polymerization (ROMP). Compared to polynorbornene, data showed that catalysts in aggregates of polyDCPD retained higher activity for longer-outcomes not directly inferable from simple diffusional-access predictions. The ability to assign catalytic activity to polymers of specific sizes, and then to determine how this activity evolves with reaction progress, support long-term goals in the development and measurement of nano-objects that possess size-dependent catalytic activity.
Chemistry 2025 ; ? (?): e02589
