Capture of nitrogen dioxide and conversion to nitric acid in a porous metal–organic framework

Jiangnan Li, Xue Han, Xinran Zhang, Alena M. Sheveleva, Yongqiang Cheng, Floriana Tuna, Eric J.L. McInnes, Laura J. McCormick McPherson, Simon J. Teat, Luke L. Daemen, Anibal J. Ramirez-Cuesta, Martin Schröder, Sihai Yang

Research output: Contribution to journalArticlepeer-review

127 Scopus citations

Abstract

Air pollution by nitrogen oxides, NOx, is a major problem, and new capture and abatement technologies are urgently required. Here, we report a metal–organic framework (Manchester Framework Material 520 (MFM-520)) that can efficiently confine dimers of NO2, which results in a high adsorption capacity of 4.2 mmol g–1 (298 K, 0.01 bar) with full reversibility and no loss of capacity over 125 cycles. Treatment of NO2@MFM-520 with water in air leads to a quantitative conversion of the captured NO2 into HNO3, an important feedstock for fertilizer production, and fully regenerates MFM-520. The confinement of N2O4 inside nanopores was established at a molecular level, and the dynamic breakthrough experiments using both dry and humid NO2 gas streams verify the excellent stability and selectivity of MFM-520 and confirm its potential for precious-metal-free deNOx technologies.

Original languageEnglish
Pages (from-to)1085-1090
Number of pages6
JournalNature Chemistry
Volume11
Issue number12
DOIs
StatePublished - Dec 1 2019

Funding

We thank EPSRC (EP/I011870, EP/P001386, EP/K038869), ERC (AdG 742041) and the Royal Society and University of Manchester for funding, and EPSRC for funding of the EPSRC National EPR Facility at Manchester. We are especially grateful to the Advanced Light Source (ALS) and Oak Ridge National Laboratory (ORNL) for access to the beamline 11.3.1 and VISION, respectively. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. Computing resources were made available through the VirtuES and the ICE-MAN projects, funded by the Laboratory Directed Research and Development program at ORNL. J.L. and X.Z. thank the China Scholarship Council for funding, and A.M.S. thanks the Russian Science Foundation (grant no. 17-73-10320) and the Royal Society of Chemistry for funding. We also thank M. A. Denecke for helpful discussions.

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