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A facile and efficient "spheridization" method is developed to produce nitrogen-enriched hierarchically porous carbon spheres of millimeters in diameter, with intricate micro-, meso- and macro-structural features. Such spheres not only show exceptional working capacity for CO2 sorption, but also satisfy practical requirements for dynamic flow in post-combustion CO2 capture. Those were achieved using co-polymerized acrylonitrile and acrylamide as the N-enriched carbon precursor, a solvent-exchange process to create hierarchically porous macro-sphere preforms, oxidization to induce cyclization of the polymer chains, and carbonization with concurrent chemical activation by KOH. The resulting carbon spheres show a relatively high CO 2 uptake of 16.7 wt% under 1 bar of CO2 and, particularly, an exceptional uptake of 9.3 wt% under a CO2 partial pressure of 0.15 bar at 25 C. Subsequent structural and chemical analyses suggest that the outstanding properties are due to highly developed microporous structures and the relatively high pyridinic nitrogen content inherited from the co-polymer precursor, incorporated within the hierarchical porous structures. ? 2014 the Partner Organisations.

Nitrogen-enriched and hierarchically porous carbon macro-spheres – ideal for large-scale CO2 capture

Nitrogen-enriched and hierarchically porous carbon macro-spheres – ideal for large-scale CO₂ capture