Hierarchical N-Doped Carbon as CO2 Adsorbent with High CO2 Selectivity from Rationally Designed Polypyrrole Precursor
Hierarchical N-Doped Carbon as CO2 Adsorbent with High CO2 Selectivity from Rationally Designed Polypyrrole Precursor
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DOI：
10.1021/jacs.5b11955
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发表时间：
2016-01-27
影响因子：
15
通讯作者：
Bao, Zhenan
中科院分区：
文献类型：
--
作者：
To, John W. F.;He, Jiajun;Bao, Zhenan
点源碳捕获和封存是二氧化碳减排组合的重要组成部分。特别是，为了降低碳捕获成本，需要具有高容量和选择性的吸附剂。尽管物理吸附剂具有再生能耗低的优点，但同时获得高容量和足够的CO2/N-2选择性仍然是一个挑战。在这里，我们报道了一种新型氮掺杂分级碳的受控合成，该碳在物理吸附碳中表现出创纪录的高亨利定律 CO2/N-2 选择性，同时具有高 CO2 吸附能力。具体来说，我们的合成涉及合理设计改性吡咯分子，该分子可以通过氢键和静电相互作用与软普朗尼克模板共组装，产生介孔，然后碳化。低温碳化和活化过程可以形成超小孔（d < 0.5 nm）并保留氮部分，这对于增强二氧化碳亲和力至关重要。此外，我们所描述的工作提供了一种策略，可以启动合理设计的多孔共轭聚合物结构和碳基材料的开发，以用于各种潜在的应用。
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/N-2 selectivity at the same time. Here, we report the controlled synthesis of a novel N-doped hierarchical carbon that exhibits record-high Henrys law CO2/N-2 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.