Cellulose Nanofibrils Endow Phase-Change Polyethylene Glycol with Form Control and Solid-to-gel Transition for Thermal Energy Storage

[Image: see text] Green energy-storage materials enable the sustainable use of renewable energy and waste heat. As such, a form-stable phase-change nanohybrid (PCN) is demonstrated to solve the fluidity and leakage issues typical of phase-change materials (PCMs). Here, we introduce the advantage of solid-to-gel transition to overcome the drawbacks of typical solid-to-liquid counterparts in applications related to thermal energy storage and regulation. Polyethylene glycol (PEG) is form-stabilized with cellulose nanofibrils (CNFs) through surface interactions. The cellulosic nanofibrillar matrix is shown to act as an organogelator of highly loaded PEG melt (85 wt %) while ensuring the absence of leakage. CNFs also preserve the physical structure of the PCM and facilitate handling above its fusion temperature. The porous CNF scaffold, its crystalline structure, and the ability to hold PEG in the PCN are characterized by optical and scanning electron imaging, infrared spectroscopy, and X-ray diffraction. By the selection of the PEG molecular mass, the lightweight PCN provides a tailorable fusion temperature in the range between 18 and 65 °C for a latent heat storage of up to 146 J/g. The proposed PCN shows remarkable repeatability in latent heat storage after 100 heating/cooling cycles as assessed by differential scanning calorimetry. The thermal regulation and light-to-heat conversion of the PCN are confirmed via infrared thermal imaging under simulated sunlight and in a thermal chamber, outperforming those of a reference, commercial insulation material. Our PCN is easily processed as a structurally stable design, including three-dimensional, two-dimensional (films), and one-dimensional (filaments) materials; they are, respectively, synthesized by direct ink writing, casting/molding, and wet spinning. We demonstrate the prospects of the lightweight, green nanohybrid for smart-energy buildings and waste heat-generating electronics for thermal energy storage and management.