Ultramicroporous carbon materials with uniform pore size accurately adjusted to the dimension of electrolyte ions or CO2 molecule are highly desirable for maximizing specific capacitance and CO2 uptake. However, efficient ways to fine‐tuning ultramicropore size at angstrom level are scarce. A completely new approach to precisely tuning carbon ultramicropore size at sub‐angstrom level is proposed herein. Due to the varying activating strength and size of the alkali ions, the ultramicropore size can be finely tuned in the range of 0.60–0.76 nm as the activation ion varies from Li+ to Cs+. The carbons prepared by direct pyrolysis of alkali salts of carboxylic phenolic resins yield ultrahigh capacitances of up to 223 F g‐1 (205 F cm‐3) in ionic liquid electrolyte, and superior CO2 uptake of 5.20 mmol g‐1 at 1.0 bar and 25 °C. Such outstanding performance of the finely tuned carbons lies in its adjustable pore size perfectly adapted to the electrolyte ions and CO2 molecule. This work paves the way for a new route to finely tuning ultramicropore size at the sub‐angstrom level in carbon materials.

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Metal−organic frameworks (MOFs), also known as coordination polymers or coordination networks (self-assembled by multidentate organic ligands and metal ions/metal clusters), are multifunctional materials, which have been widely used in the fields of sensing, catalysis, ion exchange, adsorption/separation, or gas storage since their birth. At present, MOFs are a new type of energy storage and conversion material, which are considered as one of the most promising electrode candidates as a result of their large specific surface area, adjustable pores, open metal sites, and adjustable crystal structure. Although MOFs have the above advantages, the direct utilization of pristine MOFs as electrode materials is facing great challenges, which hinder their practical application. On the basis of this, in this review, we summarize the recent development of pristine MOFs as electrode materials for supercapacitors. On the basis of the research of these pristine MOFs, the synthesis process, energy storage performance, and structural design characteristics are summarized. Finally, we focus on the future development trend of pristine MOFs.

N-doped microporous carbons with uniform ultramicropores (∼0.50 nm) are facilely prepared by direct carbonization of K(+) exchanged meta-aminophenol-formaldehyde resin. These materials give an unprecedented CO2 uptake of 1.67 mmol g(-1) at 25 °C and 0.15 bar and superior CO2-over-N2 selectivity (50 : 1).