Reversible adsorption and confinement of nitrogen dioxide within a robust porous metal-organic framework

Han, Xue; Godfrey, Harry G.W.; Briggs, Lydia; Davies, Andrew J.; Cheng, Yongqiang; Daemen, Luke L.; Sheveleva, Alena M.; Tuna, Floriana; McInnes, Eric J.L.; Sun, Junliang; Drathen, Christina; George, Michael W.; Ramirez-Cuesta, Anibal J.; Thomas, K. Mark; Schröder, Martin; Yang, Sihai

Abstract

Nitrogen dioxide (NO2) is a major air pollutant causing significant environmental and health problems. We report reversible adsorption of NO2 in a robust metal–organic framework. Under ambient conditions, MFM-300(Al) exhibits a reversible NO2 isotherm uptake of 14.1 mmol g−1, and, more importantly, exceptional selective removal of low-concentration NO2 (5,000 to <1 ppm) from gas mixtures. Complementary experiments reveal five types of supramolecular interaction that cooperatively bind both NO2 and N2O4 molecules within MFM-300(Al). We find that the in situ equilibrium 2NO2 ↔ N2O4 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 NO2 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.

Citation

Han, X., Godfrey, H. G., Briggs, L., Davies, A. J., Cheng, Y., Daemen, L. L., Sheveleva, A. M., Tuna, F., McInnes, E. J., Sun, J., Drathen, C., George, M. W., Ramirez-Cuesta, A. J., Thomas, K. M., Schröder, M., & Yang, S. (2018). Reversible adsorption and confinement of nitrogen dioxide within a robust porous metal-organic framework. Nature Materials, 17, 691-696. https://doi.org/10.1038/s41563-018-0104-7

• Journal Article Type: Article
• Acceptance Date: May 10, 2018
• Online Publication Date: Jun 11, 2018
• Publication Date: 2018-08
• Deposit Date: Jul 23, 2018
• Publicly Available Date: Dec 12, 2018
• Journal: Nature Materials
• Print ISSN: 1476-1122
• Electronic ISSN: 1476-4660
• Publisher: Nature Publishing Group
• Peer Reviewed: Peer Reviewed
• Volume: 17
• Pages: 691-696
• DOI: https://doi.org/10.1038/s41563-018-0104-7
• Public URL: https://nottingham-repository.worktribe.com/output/937228
• Publisher URL: https://www.nature.com/articles/s41563-018-0104-7#author-information
• Contract Date: Jul 23, 2018