Abstract
Natural gas is considered the cleanest and recently the most abundant fossil fuel source, yet when it is extracted from wells, it often contains 10-20 mol% carbon dioxide (20-40 wt%), which is generally vented to the atmosphere. Efforts are underway to contain this carbon dioxide at the well-head using inexpensive and non-corrosive methods. Here we report nucleophilic porous carbons are synthesized from simple and inexpensive carbon-sulphur and carbon-nitrogen precursors. Infrared, Raman and (13)C nuclear magnetic resonance signatures substantiate carbon dioxide fixation by polymerization in the carbon channels to form poly(CO2) under much lower pressures than previously required. This growing chemisorbed sulphur- or nitrogen-atom-initiated poly(CO2) chain further displaces physisorbed hydrocarbon, providing a continuous carbon dioxide selectivity. Once returned to ambient conditions, the poly(CO2) spontaneously depolymerizes, leading to a sorbent that can be easily regenerated without the thermal energy input that is required for traditional sorbents.