Lipophilic Modified Hierarchical Multiporous rGO Aerogel-Based Organic Phase Change Materials for Effective Thermal Energy Storage

In the field of thermal energy storage, organic phase change materials (PCMs) are widely used as functional materials to boost thermal applications. However, there is often a tradeoff between constructing shape-stable composite PCMs with high enthalpy value and those with low leakage rates. Here, we proposed a promising scheme to address this issue. A novel hydrogel consisting of reduced graphene oxide (rGO) and covalent organic framework (COF) was prepared via hydrothermal methods, and the rGO–COF ultralight aerogel with a hierarchical porous structure was formed after freeze-drying. The rGO–COF aerogel shows excellent absorption ability and affinity for organic solvents. It can sufficiently adsorb the molten organic PCMs, such as polyethylene glycol (PEG), and synthesize shape-stable composite PCMs with excellent leak resistance. The COF grown on the surface of rGO has a superior affinity for PEG, so rGO–COF aerogel shows an outstanding PEG loading rate of up to 96.1 wt %, which is 1.7 wt % higher than that of rGO aerogel. In addition, the COF effectively reduces the subcooling of PEG/rGO–COF with 20.3%, compared to PEG/rGO. Meanwhile, the prepared PEG/rGO–COF exhibits extremely high enthalpy and relative enthalpy efficiency (164.6 J/g, 97.4%). This demonstrates that a promising direction was highlighte for the preparation of high-enthalpy shape-stable composite organic PCMs in this work.