Selective and Regenerative Carbon Dioxide Capture by Highly Polarizing Porous Carbon Nitride

Energy-efficient CO₂ capture is a stringent demand for green and sustainable energy supply. Strong adsorption is desirable for high capacity and selective capture at ambient conditions but unfavorable for regeneration of adsorbents by a simple pressure control process. Here we present highly regenerative and selective CO₂ capture by carbon nitride functionalized porous reduced graphene oxide aerogel surface. The resultant structure demonstrates large CO₂ adsorption capacity at ambient conditions (0.43 mmol·g^–1) and high CO₂ selectivity against N₂ yet retains regenerability to desorb 98% CO₂ by simple pressure swing. First-principles thermodynamics calculations revealed that microporous edges of graphitic carbon nitride offer the optimal CO₂ adsorption by induced dipole interaction and allows excellent CO₂ selectivity as well as facile regenerability. This work identifies a customized route to reversible gas capture using metal-free, two-dimensional carbonaceous materials, which can be extended to other useful applications