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While chemical vapor deposition of diamond films is currently cost prohibitive for biosensor construction, in this paper, we show that sonication-assisted nanostructuring of biosensing electrodes with nanodiamonds (NDs) allows harnessing the hydrolytic stability of the diamond biofunctionalization chemistry for real-time continuous sensing, while improving the detector sensitivity and stability. We find that the higher surface coverages were important for improved bacterial capture and can be achieved through proper choice of solvent, ND concentration, and seeding time. A mixture of methanol and dimethyl sulfoxide provides the highest surface coverage (33.6 ± 3.4%) for the NDs with positive zeta-potential, compared to dilutions of dimethyl sulfoxide with acetone, ethanol, isopropyl alcohol, or water. Through impedance spectroscopy of ND-seeded interdigitated electrodes (IDEs), we found that the ND seeds serve as electrically conductive islands only a few nanometers apart. Also we show that the seeded NDs are amply hydrogenated to be decorated with antibodies using the UV-alkene chemistry, and higher bacterial captures can be obtained compared to our previously reported work with diamond films. When sensing bacteria from 106 cfu/mL E. coliO157:H7, the resistance to charge transfer at the IDEs decreased by ∼38.8%, which is nearly 1.5 times better than that reported previously using redox probes. Further in the case of 108 cfu/mL E. coliO157:H7, the charge transfer resistance changed by ∼46%, which is similar to the magnitude of improvement reported using magnetic nanoparticle-based sample enrichment prior to impedance detection. Thus ND seeding allows impedance biosensing in low conductivity solutions with competitive sensitivity.

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As a novel molecular and functional imaging modality, X-ray luminescence computed tomography (XLCT) has shown its potentials in biomedical and preclinic applications. However, there are still some limitations of X-ray-excited luminescent materials, such as low luminescence efficiency, poor biocompatibility, and cytotoxicity, making in vivo XLCT imaging quite challenging. In this study, for the very first time, we present on using sub-10 nm β-NaGdF:X% Eu nanoparticles with poly(acrylic acid) (PAA) surface modification, which demonstrate outstanding luminescence efficiency, uniform size distribution, water dispersity, and biosafety, as the luminescent probes for in vivo XLCT application. The pure hexagonal phase (β-) NaGdF has been successfully synthesized and characterized by X-ray powder diffraction (XRD) and transmission electron microscopy (TEM), and then the results of X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectrometry  (EDX), and elemental mapping further confirm Eu ions doped into NaGdF host. Under X-ray excitation, the β-NaGdF nanoparticles with a doping level of 15% Eu exhibited the most efficient luminescence intensity. Notably, the doping level of Eu has no effect on the crystal phase and morphology of the NaGdF-based host. Afterward, β-NaGdF:15% Eu nanoparticles were modified with PAA to enhance the water dispersity and biocompatibility. The compatibility of in vivo XLCT imaging using such nanoparticles was systematically studied via in vitro cytotoxicity, physical phantom, and in vivo imaging experiments. The ultralow cytotoxicity of PAA-modified nanoparticles, which is confirmed by over 80% cell viability of SH-SY5Y cells when treated by high nanoparticle concentration of 200 μg/mL, overcome the major obstacle for in vivo application. In addition, the high luminescence intensity of PAA-modified nanoparticles enables the location error of in vivo XLCT imaging less than 2 mm, which is comparable to that using commercially available bulk material YO:15% Eu. The proposed nanoparticles promote XLCT research into an in vivo stage. Further modification of these nanoparticles with biofunctional molecules could enable the potential of targeting XLCT imaging.