Journal
ANALYTICAL CHEMISTRY
Volume 94, Issue 5, Pages 2641-2647Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.1c05154
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Funding
- National Key Research & Development Program of China [2020YFA0709900]
- National Natural Science Foundation of China [22027805, 21804134, 62134003, 22104016]
- Major Project of Science and Technology of Fujian Province [2020HZ06006]
- Natural Science Foundation of Fujian Province [2019J05157]
- Special Funded Project of China Postdoctoral Science Foundation [2021T140117]
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By anchoring ligands, the luminescence and bioimaging capability of gold nanoclusters have been improved. The core-satellite structure of the assemblies enabled enhanced photoluminescence and prolonged blood circulation. Additionally, selective photoluminescence quenching facilitated liver imaging for H2S detection, allowing real-time evaluation of H2S delivery and prodrug screening.
Ultrasmall gold nanoclusters (AuNCs) are emerging as promising luminescent nanoprobes for bioimaging due to their fantastic photoluminescence (PL) and renal-clearable ability. However, it remains a great challenge to design them for in vivo sensitive molecular imaging in desired tissues. Herein, we have developed a strategy to tailor the PL and biofate of near-infrared II (NIR-II)emitting AuNCs via ligand anchoring for improved bioimaging. By optimizing the ligand types in AuNCs and using Er3+-doped lanthanide (Ln) nanoparticles as models, core-satellite Ln@AuNCs assemblies were rationally constructed, which enabled 2.5-fold PL enhancement of AuNCs at 1100 nm and prolonged blood circulation compared to AuNCs. Significantly, Ln@AuNCs with dual intense NIR-II PL (from AuNCs and Er3+) can effectively accumulate in the liver for ratiometric NIR-II imaging of H2S, facilitated by H2S-mediated selective PL quenching of AuNCs. We have then demonstrated the real-time imaging evaluation of liver delivery efficacy and dynamics of two H2S prodrugs. This shows a paradigm to visualize liver H2S delivery and its prodrug screening in vivo. Note that Ln@AuNCs are body-clearable via the hepatobiliary excretion pathway, thus reducing potential long-term toxicity. Such findings may propel the engineering of AuNC nanoprobes for advancing in vivo bioimaging analysis.
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