Multifunctional Reversible Self-Assembled Structures of Cellulose-Derived Phase-Change Nanocrystals

Owing to advantageous properties attributed to well-organized structures, multifunctional materials with reversible hierarchical and highly ordered arrangement in solid-state assembled structures have drawn tremendous interest. However, such materials rarely exist. Based on the reversible phase transition of phase-change materials (PCMs), phase-change nanocrystals (C18-UCNCs) are presented herein, which are capable of self-assembling into well-ordered hierarchical structures. C18-UCNCs have a core-shell structure consisting of a cellulose crystalline core that retains the basic structure and a soft shell containing octadecyl chains that allow phase transition. The distinct core-shell structure and phase transition of octadecyl chains allow C18-UCNCs to self-assemble into flaky nano/microstructures. These self-assembled C18-UCNCs exhibit efficient thermal transport and light-to-thermal energy conversion, and thus are promising for thermosensitive imaging. Specifically, flaky self-assembled nano/microstructures with manipulable surface morphology, surface wetting, and optical properties are thermoreversible and show thermally induced self-healing properties. By using phase-change nanocrystals as a novel group of PCMs, reversible self-assembled multifunctional materials can be engineered. This study proposes a promising approach for constructing self-assembled hierarchical structures by using phase-change nanocrystals and thereby significantly expands the application of PCMs.