Electronic and Thermodynamic Properties of the Amino- and Carboxamido-Functionalized C-60-Based Fullerenes: Towards Non-Volatile Carbon Dioxide Scavengers

TL;DR

This study uses computational methods to analyze amino- and carboxamido-functionalized C60 fullerenes, revealing their potential as non-volatile, thermodynamically favorable CO2 scavengers with promising applications in greenhouse gas mitigation.

Contribution

It provides a detailed theoretical characterization of functionalized fullerenes, highlighting their potential for efficient CO2 capture without the volatility issues of traditional solutions.

Findings

Polyaminofullerenes favor CO2 reaction enthalpically.

Hydration thermodynamics improve with polar group attachment.

CO2 capture free energy is insensitive to amino group count.

Abstract

Development of new greenhouse gas scavengers is actively pursued nowadays. Volatility caused solvent consumption and significant regeneration costs associated with the aqueous amine solutions motivate search for more technologically and economically advanced solutions. We hereby used hybrid density functional theory to characterize thermodynamics, structure, electronic and solvation properties of amino and carboxamido functionalized C60 fullerene. C60 is non-volatile and supports a large density of amino groups on its surface. Attachment of polar groups to fullerene C60 adjusts its dipole moment and band gap quite substantially, ultimately resulting in systematically better hydration thermodynamics. Reaction of polyaminofullerenes with CO2 is favored enthalpically, but prohibited entropically at standard conditions. Free energy of the CO2 capture by polyaminofullerenes is non-sensitive to the number of amino groups per fullerene. This result fosters consideration of polyaminofullerenes for CO2 fixation.