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Atmospheric CO 2  concentrations continue to rise rapidly in response to increased combustion of fossil fuels, contributing to global climate change. In order to mitigate the effects of global warming, development of new materials for cost-effective and energy-efficient CO 2  capture is critically important. Graphene-based porous materials are an emerging class of solid adsorbents for selectively removing CO 2  from flue gases. Herein, we report a simple and scalable approach to produce three-dimensional holey graphene frameworks with tunable porosity and pore geometry, and demonstrate their application as high-performance CO 2  adsorbents. These holey graphene macrostructures exhibit a significantly improved specific surface area and pore volume compared to their pristine counterparts, and can be effectively used in post-combustion CO 2  adsorption systems because of their intrinsic hydrophobicity together with good gravimetric storage capacities, rapid removal capabilities, superior cycling stabilities, and moderate initial isosteric heats. In addition, an exceptionally high CO 2  over N 2  selectivity can be achieved under conditions relevant to capture from the dry exhaust gas stream of a coal burning power plant, suggesting the possibility of recovering highly pure CO 2  for long-term sequestration and/or utilization for downstream applications.

Holey graphene frameworks for highly selective post-combustion carbon capture