In the global transition to a sustainable low‐carbon economy, CO2 capture and storage technology still plays a critical role for deep emission reduction, particularly for the stationary sources in power generation and industry. However, for small and mobile emission sources in transportation, CO2 capture is not suitable and it is more practical to use relatively clean energy, such as natural gas. In these two low‐carbon energy technologies, designing highly selective sorbents is one of the key and most challenging steps. Toward this end, metal‐organic frameworks (MOFs) have received continuously intensive attention in the past decades for their highly porous and diversified structures. In this review, the recent progress in developing MOFs for selective CO2 capture from post‐combustion flue gas and CH4 storage for vehicle applications are summarized. For CO2 capture, several promising strategies being used to improve CO2 adsorption uptake at low pressures are highlighted and compared. In addition, the conventional and novel regeneration techniques for MOFs are also discussed. In the case of CH4 storage, the flexible and rigid MOFs, whose CH4 storage capacity is close to the target set by U.S. Department of Energy are particularly emphasized. Finally, the challenge of using MOFs for CH4 storage is discussed.
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