Eliminating trade-offs between optical scattering and mechanical durability in aerogels as outdoor passive cooling metamaterials.

Passive cooling is a promising approach for reducing the large energy consumption to achieve carbon neutrality. Foams/aerogels can be considered effective daytime cooling materials due to their good solar scattering and thermal insulation capacity. However, the contradiction between the desired high solar reflectivity and mechanical performance still limits their scalable production and real application. Herein, inspired by the "Floor-Pillar" concept in the building industry, a multi-structure assembly-induced ice templating technology was used to construct all-cellulosic aerogels with well-defined biomimetic structures. By using cellulose nanofibers (CNFs) as pillars and cellulose nanocrystals (CNCs) as floors and methyltrimethoxysilane (MTMS) as a crosslinking material, an all-cellulosic aerogel (NCA) exhibiting high mechanical strength (mechanical strength = 0.3 MPa at 80% compression ratio, Young's modulus = 1 MPa), ultralow thermal conductivity (28 mW m K), ultrahigh solar reflectance (97.5%), high infrared emissivity (0.93), as well as excellent anti-weather function can be achieved, exceeding the performance of most reported cellulosic aerogels. Furthermore, the mechanisms of the improved mechanical strength and stimulated superior solar reflectance of NCA were studied in detail using finite element simulations and COMSOL Multiphysics. As a result, the NCA can achieve a cooling efficiency of 7.5 °C during the daytime. The building energy stimulus demonstrated that 44% of cooling energy can be saved in China annually if the NCA is applied. This work lays the foundation for the preparation of biomass aerogels for energy-saving applications.