Fossil fuels are the main contributor to global energy consumption, which has increased the amount of atmospheric CO2, increasing the severity of climate change and health issues, leading to significant interest in carbon capture. Current technologies to adsorb CO2 use liquid amines, which has led many to look for sustainable, regenerable alternatives. Recently aminosilane species, such as amino-propyl silane (APS), grafted onto a porous solid support (typically mesoporous silicas) have proven to be effective CO2 sorbents under both realistic flue-gas (10 % CO2) and direct-air-capture (400 ppm CO2) conditions. We therefore propose to explore the interactions of CO2 and supported amines using INS to understand the vibrational stretches observed and contrast them with literature FTIR data to correctly assign the data, in combination with DFT calculations performed by us.