Ultrathin Nanosheet-Supported Ag@Ag₂O Core-Shell Nanoparticles with Vastly Enhanced Photothermal Conversion...

Photothermal therapy (PTT) working in the second near-infrared (NIR-II) region has aroused a huge interest due to its potential application in terms of clinical cancer treatment. However, owing to the lack of photothermal nanoagents with high photothermal conversion efficiency, NIR-II-driven PTT still suffers from poor efficiency and subsequent cancer recurrence. In this work, we show a new and highly efficient preparation approach for NIR-II photothermal nanoagents and tailor ultrathin layered double hydroxide (LDH)-supported Ag@Ag₂O core-shell nanoparticles (Ag@Ag₂O/LDHs-U), vastly improving NIR-II photothermal performance. A combination study (high-resolution transmission electron microscopy (HRTEM), extended X-ray absorption fine structure spectroscopy (EXAFS), and X-ray photoelectron spectroscopy (XPS)) verifies that ultrafine Ag@Ag₂O core-shell nanoparticles (∼3.8 nm) are highly dispersed and firmly immobilized within ultrathin LDH nanosheets, and their Ag₂O shell possesses abundant vacancy-type defects. These unique Ag@Ag₂O/LDHs-U display an impressive photothermal conversion efficiency as high as 76.9% at 1064 nm. Such an excellent photothermal performance is likely attributed to the enhanced localized surface plasmon resonance (LSPR) coupling effect between Ag and Ag₂O and the reduced band gap caused by vacancy-type defects in the Ag₂O shell. Meanwhile, Ag@Ag₂O/LDHs-U also show prominent photothermal stability, due to the unique supported core-shell nanostructure. Moreover, both in vitro and in vivo studies further confirm that Ag@Ag₂O/LDHs-U possess good biocompatible properties and outstanding PTT therapeutic efficacy in the NIR-II region. This research shows a new strategy in the rational design and preparation of an efficient photothermal agent, which is helpful to achieve more accurate and effective cancer theranostics.