In accordance with one aspect, the present invention provides a composition which contains the amino-siloxane structures I, or III, as described herein. The composition is useful for the capture of carbon dioxide from process streams. In addition, the present invention provides methods of preparing the amino-siloxane composition. Another aspect of the present invention provides methods for reducing the amount of carbon dioxide in a process stream employing the amino-siloxane compositions of the invention, as species which react with carbon dioxide to form an adduct with carbon dioxide.