These results indicate that temperature significantly impacts the Al chemical shift, varying in the actual effect depending on the particular water content in the MFI zeolite. In models with higher water content, temperature indirectly influences the chemical shift by altering the water dynamics, which in turn affects the local environment of the aluminium atom. In dehydrated MFI, the temperature changes the local geometry of the Al-center, e.g., by weakening the intrazeolitic hydrogen bonding.