Near-Infrared II Gold Nanocluster Assemblies with Improved Luminescence and Biofate for In Vivo Ratiometric Imaging of H2S

• Published in: Analytical chemistry (Washington) Vol. 94; no. 5; pp. 2641 - 2647
• Main Authors: Li, Shihua, Ma, Qiuping, Wang, Chenlu, Yang, Kaidong, Hong, Zhongzhu, Chen, Qiushui, Song, Jibin, Song, Xiaorong, Yang, Huanghao
• Format: Journal Article
• Language: English
• Published: Washington American Chemical Society 08-02-2022
• Subjects: Analytical chemistry; Assemblies; Biocompatibility; Blood circulation; Chemistry; Erbium; Gold; Hydrogen sulfide; I.R. radiation; Ligands; Liver; Medical imaging; Nanoclusters; Nanoparticles; Near infrared radiation; Photoluminescence; Photons; Prodrugs; Toxicity
• ISSN: 0003-2700; 1520-6882
• DOI: 10.1021/acs.analchem.1c05154

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.