Sub-nm Pore Size of Phenylethynyl End-Capped Imide Oligomer-Derived Carbon for Molecular Sorption and Separation
Sub-nm Pore Size of Phenylethynyl End-Capped Imide Oligomer-Derived Carbon for Molecular Sorption and Separation
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DOI：
10.1021/acsanm.3c02516
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发表时间：
2023-08
影响因子：
5.9
通讯作者：
W. Guzman;Anthony Griffin;M. Robertson;W. Jarrett;Zhe Qiang;J. Wiggins
中科院分区：
文献类型：
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作者：
W. Guzman;Anthony Griffin;M. Robertson;W. Jarrett;Zhe Qiang;J. Wiggins
由聚合物前体衍生的碳分子筛（cms）可大规模制备，对各种节能吸附和分离技术具有吸引力，如氢气回收，空气净化和碳氢化合物分离。制备具有均匀亚纳米孔的cms是谨慎的，但研究很少。在这里，我们报告了使用苯基乙基端端交联剂来控制孔径，导致6和7之间高度均匀的孔隙形成Å。我们证明，在具有不对称化学结构的热重排（TR）亚胺低聚物中加入苯基乙基端化官能团，可以得到具有一致孔径（6-7 Å）、高表面积（高达775 m2/g）和优异的CO2吸附性能（3.17 mmol CO2/g CMS）的CMS。此外，我们的研究结果表明，亚纳米孔隙形成可以通过聚合物网络结构进一步定制，从而实现可变表面积（569-735 m2/g），这是通过控制具有或不具有TR能力的聚合物前驱体的成分来实现的。对端苯乙基聚合物前驱体的分子设计对其衍生碳结构的影响的基本理解可以为其合理设计提供关键的见解，为未来的分子吸附和分离应用提供重要的见解。
Carbon molecular sieves (CMSs) derived from polymer precursors that can be prepared at scale are attractive for various energy-efficient sorption and separation technologies, such as hydrogen recovery, air purification, and hydrocarbon separation. Preparing CMSs with uniform sub-nm pores is prudent but rarely studied. Here, we report the use of phenylethynyl-terminated crosslinkers to control pore size, leading to highly uniform pore formation between 6 and 7 Å. We demonstrate that incorporating phenylethynyl-terminated functionalities into thermally rearrangeable (TR) imide oligomers with asymmetric chemical structures results in CMSs with consistent pore sizes (6–7 Å), high surface areas (up to 775 m2/g), and excellent CO2sorption performance (3.17 mmol CO2/g of CMS). Additionally, our results indicate that sub-nm pore formation can be further tailored through polymer network architecture, leading to variable surface areas (569–735 m2/g), which is accomplished through composition control of polymer precursors with and without TR capabilities. The fundamental understandings about the impact of the molecular design of phenylethynyl-terminated polymer precursors on their derived carbon structure can provide critical insights into their rational design for future molecular sorption and separation applications.