Hydrogen Peroxide-Triggered Disassembly of Boronic Ester-Cross-Linked Brush-Arm Star Polymers
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nihms-1923400.pdf
Description
Accepted version
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1.61 MB
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Author(s)
Costa, Leticia C
Shieh, Peyton
Zafar, Hadiqa
Thiabaud, Gregory
Bobylev, Eduard O
Jasanoff, Alan
Johnson, Jeremiah A
Date Issued
August 4, 2023
Journal
ACS Macro Letters
Publisher
American Chemical Society
Citation
Leticia C. Costa, Peyton Shieh, Hadiqa Zafar, Gregory Thiabaud, Eduard O. Bobylev, Alan Jasanoff, Jeremiah A. Johnson; Hydrogen Peroxide-Triggered Disassembly of Boronic Ester-Cross-Linked Brush-Arm Star Polymers. ACS Macro Lett. 15 August 2023; 12 (8): 1179–1184.
Version
Author's final manuscript
Abstract
The concentrations of reactive oxygen species (ROS), e.g., H2O2, are often elevated in diseased tissue microenvironments. Therefore, the selective detection of ROS could enable new diagnostic methods or tools for chemical biology. Here, we report the synthesis of boronic ester-bis-norbornene core-cross-linked brush-arm star polymers (BASPs) with polyethylene glycol (PEG) or PEG-branch-spirocyclohexyl nitroxide (chex) shells. Size exclusion chromatography (SEC) and dynamic light scattering (DLS) showed that these BASPs have narrowly dispersed molar masses and average hydrodynamic diameters of 23 ± 2 nm, respectively. Moreover, due to their core–shell structures, these BASPs disassemble into bottlebrush fragments with improved selectivity for H2O2 over ROS such as peroxynitrite (ONOO–) and hypochlorite (−OCl). Finally, H2O2 induced disassembly of chex-containing BASPs induces a change in transverse magnetic relaxivity that can be detected via magnetic resonance imaging (MRI). Chex-BASPs may represent a valuable new diagnostic tool for H2O2 sensing.
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DOI of Published Version
https://doi.org/10.1021/acsmacrolett.3c00323
