Tobermorite and Al-substituted tobermorite with varying Al/(Si + Al) molar ratios were synthesized via the static hydrothermal method. The effect of different Al substitution ratios on the structure of tobermorite was investigated by XRD, SEM–EDS, TG–DSC, FT–IR, ²⁹Si, and ²⁷Al MAS–NMR. The interplanar crystal spacing of (002) increased with the increment of the Al substitution ratio. The maximum ratio of the Al substitution for Si in the structure of tobermorite was about 15 at %, which was limited by the compositions of tobermorite and the electrostatic repulsive forces caused by Al substitution. The DSC curve of the tobermorite with an Al/(Al + Si) molar ratio of 0.15 showed a larger exothermic peak area at 850 °C, indicating that the Al-O-Si bond was formed in the structure of tobermorite and the Al participated in the recrystallization. The ²⁹Si and ²⁷Al MAS–NMR results confirmed that tetrahedral Al was introduced into the structure of the tobermorite. New silicon sites, Q²(1Al) and Q³(1Al), formed by the Al substitution for Si in bridging and non-bridging sites, were detected. Compared to the tobermorite without Al substitution, the adsorption capacity of Al-substituted tobermorite with Al/(Al + Si) = 0.15 to Na⁺ was improved by 44%.

Radiative cooling is a passive cooling technology that can cool a space without any external energy by reflecting sunlight and radiating heat to the universe. Current reported radiative cooling techniques can present good outside test results, however, manufacturing an efficient radiative material which can be applied to the market for large-scale application is still a huge challenge. Here, an effective radiative cooling coating with a near-ideal selective emissive spectrum is prepared based on the molecular vibrations of SiO_x, mica, rare earth silicate, and molybdate functional nanoparticles. The radiative cooling coating can theoretically cool 45 °C below the ambient temperature in the nighttime. Polyethylene terephthalate (PET) aluminized film was selected as the coating substrate for its flexibility, low cost, and extensive production. As opposed to the usual investigations that measure the substrate temperature, the radiative cooling coating was made into a cubic box to test its space cooling performance on a rooftop. Results showed that a temperature reduction of 4 ± 0.5 °C was obtained in the nighttime and 1 ± 0.2 °C was achieved in the daytime. Furthermore, the radiative cooling coating is resistant to weathering, fouling, and ultraviolet radiation, and is capable of self-cleaning due to its hydrophobicity. This practical coating may have a significant impact on global energy consumption.