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Hierarchical N-Doped Carbon as CO2 Adsorbent with High CO2 Selectivity from Rationally Designed Polypyrrole Precursor

To, John W. F., He, Jiajun, Mei, Jianguo, Haghpanah, Reza, Chen, Zheng, Kurosawa, Tadanori, Chen, Shucheng, Bae, Won-Gyu, Pan, Lijia, Tok, Jeffrey B.-H., Wilcox, Jennifer, Bao, Zhenan
Journal of the American Chemical Society 2016 v.138 no.3 pp. 1001-1009
adsorbents, adsorption, carbon, carbon dioxide, carbon sequestration, carbonization, electrostatic interactions, energy, greenhouse gas emissions, hydrogen bonding, nitrogen, polymers
Carbon capture and sequestration from point sources is an important component in the CO₂ emission mitigation portfolio. In particular, sorbents with both high capacity and selectivity are required for reducing the cost of carbon capture. Although physisorbents have the advantage of low energy consumption for regeneration, it remains a challenge to obtain both high capacity and sufficient CO₂/N₂ selectivity at the same time. Here, we report the controlled synthesis of a novel N-doped hierarchical carbon that exhibits record-high Henry’s law CO₂/N₂ selectivity among physisorptive carbons while having a high CO₂ adsorption capacity. Specifically, our synthesis involves the rational design of a modified pyrrole molecule that can co-assemble with the soft Pluronic template via hydrogen bonding and electrostatic interactions to give rise to mesopores followed by carbonization. The low-temperature carbonization and activation processes allow for the development of ultrasmall pores (d < 0.5 nm) and preservation of nitrogen moieties, essential for enhanced CO₂ affinity. Furthermore, our described work provides a strategy to initiate developments of rationally designed porous conjugated polymer structures and carbon-based materials for various potential applications.