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

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• 作者：John W. F. To ; Jiajun He ; Jianguo Mei ; Reza Haghpanah ; Zheng Chen ; Tadanori Kurosawa ; Shucheng Chen ; Won-Gyu Bae ; Lijia Pan ; Jeffrey B.-H. Tok ; Jennifer Wilcox ; Zhenan Bao
• 刊名：Journal of the American Chemical Society
• 出版年：2016
• 出版时间：January 27, 2016
• 年：2016
• 卷：138
• 期：3
• 页码：1001-1009
• 全文大小：594K
• ISSN：1520-5126

文摘

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.