Fluorescence Quenching of Carbon Nitride Nanosheet through Its Interaction with DNA for Versatile Fluorescence Sensing

This work investigates the interaction of carbon nitride nanosheet (CNNS), a recently developed two-dimensional nanomaterial, with DNA and its fluorescence quenching mechanism on fluorophore labeled single-stranded DNA probes. The static quenching through the photoinduced electron transfer (PET) from the excited fluorophore to the conductive band of CNNS is identified. Utilizing the affinity change of CNNS to DNA probes upon their recognition to targets and the PET-based fluorescence quenching effect, a universal sensing strategy is proposed for design of several homogeneous fluorescence detection methods with short assay time and high sensitivity. This strategy is versatile and can be combined with different amplification tools for quick fluorescence sensing of DNA and extensive DNA related analytes such as metal cations, small molecules, and proteins. As examples, two simple fluorescence detection methods for DNA and Hg²⁺, one facile detection method coupled with Exo III-mediated target recycling for sensitive DNA analysis, and a ratiometric fluorescence protocol for DNA detection are proposed. This work provides an avenue for understanding the interaction between two-dimensional nanomaterials and biomolecules and designing novel sensing strategies for extending the applications of nanomaterials in bioanalysis

Folate Receptor-Targeted and Cathepsin B‑Activatable Nanoprobe for <i>In Situ</i> Therapeutic Monitoring of Photosensitive Cell Death

The integration of diagnostic and therapeutic functions in a single system holds great promise to enhance the theranostic efficacy and prevent the under- or overtreatment. Herein, a folate receptor-targeted and cathepsin B-activatable nanoprobe is designed for background-free cancer imaging and selective therapy. The nanoprobe is prepared by noncovalently assembling phospholipid-poly­(ethylene oxide) modified folate and photosensitizer-labeled peptide on the surface of graphene oxide. After selective uptake of the nanoprobe into lysosome of cancer cells via folate receptor-mediated endocytosis, the peptide can be cleaved to release the photosensitizer in the presence of cancer-associated cathepsin B, which leads to 18-fold fluorescence enhancement for cancer discrimination and specific detection of intracellular cathepsin B. Under irradiation, the released photosensitizer induces the formation of cytotoxic singlet oxygen for triggering photosensitive lysosomal cell death. After lysosomal destruction, the lighted photosensitizer diffuses from lysosome into cytoplasm, which provides a visible method for <i>in situ</i> monitoring of therapeutic efficacy. The nanoprobe exhibits negligible dark toxicity and high phototoxicity with the cell mortality rate of 0.06% and 72.1%, respectively, and the latter is specific to folate receptor-positive cancer cells. Therefore, this work provides a simple but powerful protocol with great potential in precise cancer imaging, therapy, and therapeutic monitoring

Surface Decorated Porphyrinic Nanoscale Metal–Organic Framework for Photodynamic Therapy

Nanocrystallization of organic molecular photosensitizers (PSs) by means of NMOF platforms has been demonstrated to be a promising approach to build up highly efficient PDT therapeutics. We report herein a new UiO-66 type of NMOF-based PS (<b>UiO-66-TPP-SH</b>), which is generated from UiO-66 NMOF and S-ethylthiol ester monosubstituted metal free porphyrin (<b>TPP-SH</b>) via a facile postsynthetic approach under mild conditions. The obtained NMOF (size less than 150 nm) with surface-decorated porphyrinic PS can not only retain MOF crystallinity, structural feature, and size, but also exhibit highly efficient singlet oxygen generation. Compared to the interior-located porphyrinic NMOF, <b>UiO-66-TPP-SH</b> shows significantly higher photodynamic activity and more efficient PDT tumor treatment