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, Yang Sihai, Schröder Martin
School of Chemistry, University of Manchester, Manchester, UK.
School of Chemistry, University of Nottingham, Nottingham, UK.
Nat Mater. 2018 Aug;17(8):691-696. doi: 10.1038/s41563-018-0104-7. Epub 2018 Jun 11.
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.
二氧化氮（NO）是一种主要的空气污染物，会引发严重的环境和健康问题。我们报道了在一种坚固的金属有机框架中NO的可逆吸附。在环境条件下，MFM-300（Al）表现出14.1 mmol g的可逆NO等温线吸附量，更重要的是，它能从气体混合物中出色地选择性去除低浓度NO（5000至<1 ppm）。补充实验揭示了五种超分子相互作用，它们协同结合MFM-300（Al）内的NO和NO分子。我们发现，孔内原位平衡2NO ↔ NO与压力无关，而异位时这种平衡是典型的压力依赖性一级过程。MFM-300（Al）中NO的螺旋单体 - 二聚体链的共存可为深入理解多孔主体内客体分子的化学性质提供基础。这项工作可能为未来捕获和转化技术的发展铺平道路。
