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

被引:191
作者
Han, Xue [1 ]
Godfrey, Harry G. W. [1 ]
Briggs, Lydia [1 ]
Davies, Andrew J. [2 ]
Cheng, Yongqiang [3 ]
Daemen, Luke L. [3 ]
Sheveleva, Alena M. [1 ,4 ,5 ]
Tuna, Floriana [1 ]
Mcinnes, Eric J. L. [1 ]
Sun, Junliang [6 ]
Drathen, Christina [7 ]
George, Michael W. [2 ,8 ]
Ramirez-Cuesta, Anibal J. [3 ]
Thomas, K. Mark [9 ]
Yang, Sihai [1 ]
Schroder, Martin [1 ]
机构
[1] Univ Manchester, Sch Chem, Manchester, Lancs, England
[2] Univ Nottingham, Sch Chem, Nottingham, England
[3] Oak Ridge Natl Lab, Chem & Engn Mat Div, Neutron Sci Directorate, Oak Ridge, TN USA
[4] Int Tomog Ctr SB RAS, Novosibirsk, Russia
[5] Novosibirsk State Univ, Novosibirsk, Russia
[6] Peking Univ, Coll Chem & Mol Engn, Beijing, Peoples R China
[7] European Synchrotron Radiat Facil, Grenoble, France
[8] Univ Nottingham Ningbo China, Dept Chem & Environm Engn, Ningbo, Zhejiang, Peoples R China
[9] Univ Newcastle Tyne, Sch Chem Engn & Adv Mat, Northern Carbon Res Labs, Newcastle Upon Tyne, Tyne & Wear, England
基金
英国工程与自然科学研究理事会; 俄罗斯科学基金会;
关键词
AMBIENT CONDITIONS; DINITROGEN TETROXIDE; NO2; ADSORPTION; ADSORBENTS; REMOVAL; DIFFRACTION; POLLUTION; PRESSURE; SOFTWARE; CAPACITY;
D O I
10.1038/s41563-018-0104-7
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nitrogen dioxide (NO2) is a major air pollutant causing significant environmental(1,2) and health problems(3,4). 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 2NO(2)<-> 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.
引用
收藏
页码:691 / +
页数:8
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