CO2 evolution is one of the urgent global issues; meanwhile, understanding of sorptive/dynamic behavior is crucial to create next-generation encapsulant materials with stable sorbent processes. Herein, we showcase molecular CO2 storage constructed by a [60]fullerenol nanopocket. The CO2 density reaches 2.401 g/cm3 within the nanopore, showing strong intramolecular interactions, which induce nanoconfinement effects such as forbidden translation, restricted rotation, and perturbed vibration of CO2. We also disclosed an equation of state for a molecular CO2 gas, revealing a very low pressure of 3.14 rPa (1 rPa = 10-27 Pa) generated by the rotation/vibration at 300 K. Curiously enough, the CO2 capture enabled to modulate an external property of the encapulant material itself, i.e., association of the [60]fullerenol via intercage hydrogen-bonding.
© 2024 The Authors. Published by American Chemical Society.