Self‐Pillared Ultramicroporous Carbon Nanoplates for Selective Separation of CH4/N2

• Published in: Angewandte Chemie International Edition 2021-03, Vol.60 (12), p.6339-6343
• Main Authors: Xu, Shuang, Li, Wen‐Cui, Wang, Cheng‐Tong, Tang, Lei, Hao, Guang‐Ping, Lu, An‐Hui
• Format: Article
• Language: English
• Subjects: Carbon; carbon nanoplates; CH4/N2 separation; Chemical synthesis; Diffusion rate; Heterostructures; hierarchical structures; Methane; Molecular sieves; Partial pressure; Polymers; porous carbon nanomaterials; Selectivity; self-assembly; Separation; Thickness
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202014231

There is growing evidence that pillaring up a densely packed ultramicroporous two‐dimensional (2D) structure is an effective strategy to reduce their internal diffusion. Reliable pillaring paradigms, however, is rather challenging. Here we report a one‐pot multi‐component sequential assembly method for the preparation of a new self‐pillared 2D polymer and ultramicroporous carbon with integrated surface protrusions. The molecular level pillaring process is surprisingly fast, that is, in 10 min. The thickness of nanoplate edge and the density (roughness), angle as well as height of protrusions can be precisely tuned. Exemplified in coal bed methane purification/separation, this unique pillared 2D carbons exhibit a CH4/N2 selectivity up to 24 at a low CH4 partial pressure and two orders of magnitude faster CH4 diffusion kinetics than the commercial carbon molecular sieves. This solution synthesis methodology is generalizable for creation and fine tuning of pillared 2D heterostructures. Self‐pillared ultramicroporous carbon nanoplates have been prepared via a one‐pot multi‐component sequential condensation, which exhibit a high selectivity and fast diffusion kinetics for CH4/N2 separation.