Temperature-Regulated Core Swelling and Asymmetric Shrinkage for Tunable Yolk@Shell Polydopamine@Mesoporous Silica Nanostructures

Facile and controllable synthesis of functional yolk@shell structured nanospheres with a tunable inner core (‘yolk') and mesoporous shell is highly desirable, yet it remains a great challenge. Herein, xx developed a strategy based on temperature-regulated swelling and restricted asymmetric shrinkage of polydopamine (PDA) nanospheres, combined with heterogeneous interface self-assembly growth. This method allows a simple and versatile preparation of PDA@mesoporous silica (MS) nanospheres exhibiting tunable yolk@shell architectures and shell pore sizes. Through reaction temperature-regulated swelling degree and confined shrinkage of PDA nanospheres, the volume ratio of the hollow cavity that the PDA core occupies can easily be tuned from ca. 2/3 to ca. 1/2, then to ca. 2/5, finally to ca. 1/3. Owing to the presence of PDA with excellent photothermal conversion capacity, the PDA@MS nanocomposites with asymmetric yolk distributions can become a colloidal nanomotor propelled by near-infrared (NIR) light. Noteworthily, the PDA@MS with half PDA yolk and microcracks in silica shell reaches 2.18 µm ² s ⁻¹ of effective diffusion coefficient (De) in the presence of 1.0 W cm ⁻² NIR light. This temperature-controlled swelling approach may provide new insight into the design and facile preparation of functional PDA-based yolk@shell structured nanocomposites for wide applications in biology and medicine.