Surface Modification of Exfoliated Layered Gadolinium Hydroxide for the Development of Multimodal Contrast Agents for MRI and Fluorescence Imaging

A novel method for modifying the surface of magnetic‐resonance‐contrasting layered gadolinium hydroxide (LGdH) is developed providing them with water‐ and bio‐compatibility and acid‐resistance, all of which are essential for medical applications. A stable colloid of exfoliated layers is synthesized by exchanging interlayer anions of LGdH with oleate ions. The delaminated layers are successively coated with phospholipids with poly(ethylene glycol) tail groups, and their effectiveness as a contrast agent for magnetic resonance imaging (MRI) is demonstrated. The adaptability of this surface modification approach for incorporating functional molecules and fabricating a fluorescent colloid of LGdH, which has the potential utility as a multimodal probe, is also demonstrated. This result provides a novel approach for expanding the applications of layered inorganic materials and developing a new class of MRI contrast agents. A stable colloid of fluorescent layered gadolinium hydroxide (LGdH) is synthesized using the newly developed surface modification method comprising the following steps: layer exfoliation, anion exchange, and coating with polyethyleneglycol. The efficient contrast‐enhancement of modified LGdH in in‐vitro and in‐vivo magnetic resonance imaging demonstrates their potential utility as a multimodal probe combining optical and magnetic resonance imaging.