Journal
NANOSCALE
Volume 10, Issue 43, Pages 20279-20288Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8nr06968a
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Funding
- National Key R & D Program of China [2017YFC0107400, 2017YFC0107401, 2017YFC0107405]
- National Natural Science Foundation of China [11804214, 81771972, 21641001]
- Natural Science Foundation of Shaanxi Province [2017JQ2020, 2017JQ8049]
- Fundamental Research Funds for the Central Universities [GK201703028, GK201701007, 2017CSY033, 2018CSLZ009]
- State Key Laboratory of Cancer Biology Fund [CBSKL201706, CBSKL2017Z05]
- China Scholarship Council (CSC) [201607845015]
- Wen-feng High-end Talents Project of Chongqing University of Posts and Telecommunications [W2016-01]
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To date, lanthanide-doped upconversion nanoparticles (UCNPs) have been widely reported as a promising CT contrast agent because they have high atomic numbers and big X-ray attenuation coefficient values. However, it is still a challenge to fabricate a simple multimodal imaging probe with improved image quality for early cancer diagnosis in clinical medicine. Herein, ultra-small, uniform and monodisperse -NaGdF4:Yb,Er,X% Lu (X = 0, 1, 2.5, 4, 6, 7.5) UCNPs were prepared through a solvothermal method with high-level modulation of both the phase and morphology. Meanwhile, a remarkably enhanced red upconversion luminescence (UCL) in the -NaGdF4:Yb,Er,X% Lu NPs was successfully realized via Lu3+ doping. It is found that as the content of Lu3+ increases from 0 to 7.5 mol%, the UCL intensity of the red emission first increases and then decreases, with the optimum doping content of Lu3+ ions of 2.5 mol%. The red UCL enhancement is ascribed to the change of the Yb-Er interionic distance controlling the Yb-Er energy transfer rate and the distortion of the local environment of Er3+ ions influencing the 4f-4f transition rates of Er3+ ions, which has been further confirmed by the experimental check of the crystallographic phase and by photoluminescence spectroscopy employing Eu3+ as the structural probe, respectively. More importantly, after being modified with the HS-PEG(2000)-NH2 ligand, the NH2-PEGylated-NaGdF4:Yb,Er,X% Lu NPs exhibited low cytotoxicity, high biocompatibility, and remarkably enhanced contrast performance in in vitro UCL and in vivo CT imaging. On the basis of our findings, the as-obtained functionalized UCNPs could be considered as a promising versatile dual-mode imaging probe for bioimaging, tumor diagnosis, and cancer therapy.
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