Rational design for enhancing inflammation-responsive in vivo chemiluminescence via nanophotonic energy relay to near-infrared AIE-active conjugated polymer

Young Hun Seo, Ajay Singh, Hong Jun Cho, Youngsun Kim, Jeongyun Heo, Chang Keun Lim, Soo Young Park, Woo Dong Jang, Sehoon Kim

Research output: Contribution to journalArticlepeer-review

41 Citations (Scopus)

Abstract

H2O2-specific peroxalate chemiluminescence is recognized as a potential signal for sensitive in vivo imaging of inflammation but the effect of underlying peroxalate-emitter energetics on its efficiency has rarely been understood. Here we report a simple nanophotonic way of boosting near-infrared chemiluminescence with no need of complicated structural design and synthesis of an energetically favored emitter. The signal enhancement was attained from the construction of a nanoparticle imaging probe (∼26 nm in size) by dense nanointegration of multiple molecules possessing unique photonic features, i.e., i) a peroxalate as a chemical fuel generating electronic excitation energy in response to inflammatory H2O2, ii) a low-bandgap conjugated polymer as a bright near-infrared emitter showing aggregation-induced emission (AIE), and iii) an energy gap-bridging photonic molecule that relays the chemically generated excitation energy to the emitter for its efficient excitation. From static and kinetic spectroscopic studies, a green-emissive BODIPY dye has proven to be an efficient relay molecule to bridge the energy gap between the AIE polymer and the chemically generated excited intermediate of H2O2–reacted peroxalates. The energy-relayed nanointegration of AIE polymer and peroxalate in water showed a 50-times boosted sensing signal compared to their dissolved mixture in THF. Besides the high H2O2 detectability down to 10−9 M, the boosted chemiluminescence presented a fairly high tissue penetration depth (>12 mm) in an ex vivo condition, which enabled deep imaging of inflammatory H2O2 in a hair-covered mouse model of peritonitis.

Original languageEnglish
Pages (from-to)111-118
Number of pages8
JournalBiomaterials
Volume84
DOIs
Publication statusPublished - 2016 Apr 1

Bibliographical note

Funding Information:
This work was supported by grants from the National Research Foundation of Korea ( 2014M3A9E5073316 , 2012K1A1A2A01055811 , and 2007-00093 ), the Korea Health Industry Development Institute ( HI15C1540 ), and the Intramural Research Program of KIST .

All Science Journal Classification (ASJC) codes

  • Bioengineering
  • Ceramics and Composites
  • Biophysics
  • Biomaterials
  • Mechanics of Materials

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