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

Authors
  • Seo, Young Hun1
  • Singh, Ajay2
  • Cho, Hong-Jun2
  • Kim, Youngsun2
  • Heo, Jeongyun3
  • Lim, Chang-Keun2
  • Park, Soo Young4
  • Jang, Woo-Dong5
  • Kim, Sehoon6
  • 1 Center for Theragnosis, Korea Institute of Science and Technology (KIST), 39-1, Hawolgok-dong, Seongbuk-gu, Seoul 136-791, Republic of Korea; Department of Chemistry, Yonsei University, 50 Yonsei-ro, Seodaemungu, Seoul 120-749, Republic of Korea. , (North Korea)
  • 2 Center for Theragnosis, Korea Institute of Science and Technology (KIST), 39-1, Hawolgok-dong, Seongbuk-gu, Seoul 136-791, Republic of Korea. , (North Korea)
  • 3 Center for Theragnosis, Korea Institute of Science and Technology (KIST), 39-1, Hawolgok-dong, Seongbuk-gu, Seoul 136-791, Republic of Korea; Department of Material Science and Engineering, Seoul National University, 599 Gwanak-ro, Gwanak-gu, Seoul 151-744, Republic of Korea. , (North Korea)
  • 4 Department of Material Science and Engineering, Seoul National University, 599 Gwanak-ro, Gwanak-gu, Seoul 151-744, Republic of Korea. , (North Korea)
  • 5 Department of Chemistry, Yonsei University, 50 Yonsei-ro, Seodaemungu, Seoul 120-749, Republic of Korea. , (North Korea)
  • 6 Center for Theragnosis, Korea Institute of Science and Technology (KIST), 39-1, Hawolgok-dong, Seongbuk-gu, Seoul 136-791, Republic of Korea. Electronic address: [email protected] , (North Korea)
Type
Published Article
Journal
Biomaterials
Publication Date
Apr 01, 2016
Volume
84
Pages
111–118
Identifiers
DOI: 10.1016/j.biomaterials.2016.01.038
PMID: 26826300
Source
Medline
Keywords
License
Unknown

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.

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