With the increasing levels of anthropogenic carbon dioxide emissions, the need for climate change mitigation has never been more urgent. Developing mass scalable, efficient, and affordable decarbonization technology is a key objective for this generation of scientists. Existing methods for CO2 removal are facilitated by thermally driven systems and thus suffer from being energy-intensive and inefficient. Joint efforts between computational and experimental chemistry fields can help steer research toward uncovering valuable insight into CO2 reactivity with the ideal sorbent. This dissertation presents an investigation into various chemical systems studied with the original objective of carbon capture and concentration and with the eventual outcome of understanding the limitations of chemistry.