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

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. Here, 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.

Authors:
 [1];  [1];  [1];  [2];  [3];  [1]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [4];  [3]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of Manchester, Manchester (United Kingdom)
  2. Univ. of Manchester, Manchester (United Kingdom); International Tomography Centre SB RAS and Novosibirsk State Univ., Novosibirsk (Russia)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1580418
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Chemistry
Additional Journal Information:
Journal Volume: 11; Journal Issue: 12; Journal ID: ISSN 1755-4330
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Li, Jiangnan, Han, Xue, Zhang, Xinran, Sheveleva, Alena M., Cheng, Yongqiang, Tuna, Floriana, McInnes, Eric J. L., McCormick McPherson, Laura J., Teat, Simon J., Daemen, Luke L., Ramirez-Cuesta, Anibal J., Schröder, Martin, and Yang, Sihai. Capture of nitrogen dioxide and conversion to nitric acid in a porous metal–organic framework. United States: N. p., 2019. Web. doi:10.1038/s41557-019-0356-0.
Li, Jiangnan, Han, Xue, Zhang, Xinran, Sheveleva, Alena M., Cheng, Yongqiang, Tuna, Floriana, McInnes, Eric J. L., McCormick McPherson, Laura J., Teat, Simon J., Daemen, Luke L., Ramirez-Cuesta, Anibal J., Schröder, Martin, & Yang, Sihai. Capture of nitrogen dioxide and conversion to nitric acid in a porous metal–organic framework. United States. https://doi.org/10.1038/s41557-019-0356-0
Li, Jiangnan, Han, Xue, Zhang, Xinran, Sheveleva, Alena M., Cheng, Yongqiang, Tuna, Floriana, McInnes, Eric J. L., McCormick McPherson, Laura J., Teat, Simon J., Daemen, Luke L., Ramirez-Cuesta, Anibal J., Schröder, Martin, and Yang, Sihai. Fri . "Capture of nitrogen dioxide and conversion to nitric acid in a porous metal–organic framework". United States. https://doi.org/10.1038/s41557-019-0356-0. https://www.osti.gov/servlets/purl/1580418.
@article{osti_1580418,
title = {Capture of nitrogen dioxide and conversion to nitric acid in a porous metal–organic framework},
author = {Li, Jiangnan and Han, Xue and Zhang, Xinran and Sheveleva, Alena M. and Cheng, Yongqiang and Tuna, Floriana and McInnes, Eric J. L. and McCormick McPherson, Laura J. and Teat, Simon J. and Daemen, Luke L. and Ramirez-Cuesta, Anibal J. and Schröder, Martin and Yang, Sihai},
abstractNote = {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. Here, 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.},
doi = {10.1038/s41557-019-0356-0},
journal = {Nature Chemistry},
number = 12,
volume = 11,
place = {United States},
year = {Fri Nov 22 00:00:00 EST 2019},
month = {Fri Nov 22 00:00:00 EST 2019}
}

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