Contamination of heavy metal ions in an aquatic environment poses a serious threat to human health. More seriously, heavy metal ions are usually present in the environment in a mixture, and the synergetic toxicity of multiple heavy metal ions is revealed (Aragay et al. Chem. Rev. 2011, 111, 3433; Chu et al. Aquat. Toxicol. 2002, 61, 53). Unfortunately, most of the existing methods based on DNA sequences are focusing on the detection of one type of metal ions. Simple and multiplexed detection of multiple metal ions has been poorly investigated and remains challenging. Here, we re-engineered the DNA sequences for Pb2+, Hg2+, and Ag+, through which the binding of multiple metal ions initiated the self-assembly of these DNA sequences. On the basis of our rationally designed multicolor fluorescent labeling of the DNA sequences, cascade fluorescence resonance energy transfer (FRET) occurred. As a result, a fingerprint fluorescent spectrum was produced to indicate the presence of a single type of metal ions or multiple metal ions. The major advantages of our cascade FRET fingerprint technology include the following: (1) the “mix and read” detection mode in homogeneous solution is simple without the need of complicated instruments; (2) only single excitation is required to provide the cascade FRET fingerprint spectrum; (3) multiplexed detection capability can be realized intuitively and sensitively.
Jing Ruan,Fang Li,Hao Tian,Jie Yu,Hongpei Deng,Shengfang Ge,Kam W. Leong
Photodynamic therapy (PDT) relies on the generation of cytotoxic singlet oxygen ( 1 O 2 ) from an otherwise nontoxic photosensitizer accumulated in tumor tissue to treat cancer. However, PDT of uveal melanoma, the most common adult intraocular cancer, using potent porphyrin derivatives as photosensitizers has shown limited therapeutic efficacy due to low bioavailability and 1 O 2 yield. Here, considering the uveal melanoma microenvironment of endogenous melanin , which has a high absorption between 300 nm and 500 nm, we design a carbon dot-based photosensitizer that uses multiple different pathways to generate 1 O 2 . We conjugated gadolinium (Gd)-doped carbon dots (Gd@Cdots) with the porphyrin-derivatives chlorin e6 (Ce6) and verteporfin (Ver). The resulting nanoparticle (Gd@Cdots/Ce6/Ver) generates 1 O 2 under UV irradiation mainly in cascade FRET from Gd@Cdots to Ce6 and then to Ver; the photoactivated Ver, in turn, transfers its energy to 3 O 2 to generate 1 O 2 . In human uveal melanoma MUM-2B cells in vitro, Gd@Cdots/Ce6/Ver generated 7.1- and 2.4-fold higher production of hydroxyl radical (·OH) and superoxide anions (O 2 - ·) following UV irradiation than Gd@Cdots, indicating greater induction of tumor cell apoptosis. In an orthotopic mouse model of uveal melanoma, PDT with Gd@Cdots/Ce6/Ver showed the same trend of superior potency in tumor growth inhibition. This photosensitizer design improves the PDT efficacy of uveal melanoma by enhancing the production of 1 O 2 and should be of broad utility to other PDT.
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