Nitrogen dioxide (NO) is a major air pollutant causing significant environmental and health problems. We report reversible adsorption of NO in a robust metal-organic framework. Under ambient conditions, MFM-300(Al) exhibits a reversible NO isotherm uptake of 14.1 mmol g, and, more importantly, exceptional selective removal of low-concentration NO (5,000 to <1 ppm) from gas mixtures. Complementary experiments reveal five types of supramolecular interaction that cooperatively bind both NO and NO molecules within MFM-300(Al). We find that the in situ equilibrium 2NO ↔ NO within the pores is pressure-independent, whereas ex situ this equilibrium is an exemplary pressure-dependent first-order process. The coexistence of helical monomer-dimer chains of NO in MFM-300(Al) could provide a foundation for the fundamental understanding of the chemical properties of guest molecules within porous hosts. This work may pave the way for the development of future capture and conversion technologies.

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