The atmospheric CO2 concentration continues a rapid increase to its current record high value of 416 ppm for the time being. It calls for advanced CO2 capture technologies. One of the attractive technologies is physical adsorption‐based separation, which shows easy regeneration and high cycle stability, and thus reduced energy penalties and cost. The extensive research on this topic is evidenced by the growing body of scientific and technical literature. The progress spans from the innovation of novel porous adsorbents to practical separation practices. Major CO2 capture materials include the most widely used industrially relevant porous carbons, zeolites, activated alumina, mesoporous silica, and the newly emerging metal‐organic frameworks (MOFs) and covalent‐organic framework (COFs). The key intrinsic properties such as pore structure, surface chemistry, preferable adsorption sites, and other structural features that would affect CO2 capture capacity, selectivity, and recyclability are first discussed. The industrial relevant variables such as particle size of adsorbents, the mechanical strength, adsorption heat management, and other technological advances are equally important, even more crucial when scaling up from bench and pilot‐scale to demonstration and commercial scale. Therefore, we aim to bring a full picture of the adsorption‐based CO2 separation technologies, from adsorbent design, intrinsic property evaluation to performance assessment not only under ideal equilibrium conditions but also in realistic pressure swing adsorption processes.

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.

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