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Synthesis of Nitro Compounds from Nitrogen Dioxide Captured in a Metal-Organic Framework

[Image: see text] Increasing levels of air pollution are driving the need for the development of new processes that take “waste-to-chemicals”. Herein, we report the capture and conversion under ambient conditions of a major air pollutant, NO(2), using a robust metal-organic framework (MOF) material,...

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Autores principales: Li, Jiangnan, Wang, Zi, Chen, Yinlin, Cheng, Yongqiang, Daemen, Luke L., Tuna, Floriana, McInnes, Eric J. L., Day, Sarah J., Ramirez-Cuesta, Anibal J., Schröder, Martin, Yang, Sihai
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9585588/
https://www.ncbi.nlm.nih.gov/pubmed/36198137
http://dx.doi.org/10.1021/jacs.2c07283
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author Li, Jiangnan
Wang, Zi
Chen, Yinlin
Cheng, Yongqiang
Daemen, Luke L.
Tuna, Floriana
McInnes, Eric J. L.
Day, Sarah J.
Ramirez-Cuesta, Anibal J.
Schröder, Martin
Yang, Sihai
author_facet Li, Jiangnan
Wang, Zi
Chen, Yinlin
Cheng, Yongqiang
Daemen, Luke L.
Tuna, Floriana
McInnes, Eric J. L.
Day, Sarah J.
Ramirez-Cuesta, Anibal J.
Schröder, Martin
Yang, Sihai
author_sort Li, Jiangnan
collection PubMed
description [Image: see text] Increasing levels of air pollution are driving the need for the development of new processes that take “waste-to-chemicals”. Herein, we report the capture and conversion under ambient conditions of a major air pollutant, NO(2), using a robust metal-organic framework (MOF) material, Zr-bptc (H(4)bptc = 3,3′,5,5′-biphenyltetracarboxylic acid), comprising {Zr(6)(μ(3)-O)(4)(μ(3)-OH)(4)(COO)(12)} clusters linked by 4-connected bptc(4–) ligands in an ftw topology. At 298 K, Zr-bptc shows exceptional stability and adsorption of NO(2) at both low (4.9 mmol g(–1) at 10 mbar) and high pressures (13.8 mmol g(–1) at 1.0 bar), as measured by isotherm experiments. Dynamic breakthrough experiments have confirmed the selective retention of NO(2) by Zr-bptc at low concentrations under both dry and wet conditions. The immobilized NO(2) can be readily transformed into valuable nitro compounds relevant to construction, agrochemical, and pharmaceutical industries. In situ crystallographic and spectroscopic studies reveal strong binding interactions of NO(2) to the {Zr(6)(μ(3)-O)(4)(μ(3)-OH)(4)(COO)(12)} cluster node. This study paves a circular pathway to enable the integration of nitrogen-based air pollutants into the production of fine chemicals.
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spelling pubmed-95855882022-10-22 Synthesis of Nitro Compounds from Nitrogen Dioxide Captured in a Metal-Organic Framework Li, Jiangnan Wang, Zi Chen, Yinlin Cheng, Yongqiang Daemen, Luke L. Tuna, Floriana McInnes, Eric J. L. Day, Sarah J. Ramirez-Cuesta, Anibal J. Schröder, Martin Yang, Sihai J Am Chem Soc [Image: see text] Increasing levels of air pollution are driving the need for the development of new processes that take “waste-to-chemicals”. Herein, we report the capture and conversion under ambient conditions of a major air pollutant, NO(2), using a robust metal-organic framework (MOF) material, Zr-bptc (H(4)bptc = 3,3′,5,5′-biphenyltetracarboxylic acid), comprising {Zr(6)(μ(3)-O)(4)(μ(3)-OH)(4)(COO)(12)} clusters linked by 4-connected bptc(4–) ligands in an ftw topology. At 298 K, Zr-bptc shows exceptional stability and adsorption of NO(2) at both low (4.9 mmol g(–1) at 10 mbar) and high pressures (13.8 mmol g(–1) at 1.0 bar), as measured by isotherm experiments. Dynamic breakthrough experiments have confirmed the selective retention of NO(2) by Zr-bptc at low concentrations under both dry and wet conditions. The immobilized NO(2) can be readily transformed into valuable nitro compounds relevant to construction, agrochemical, and pharmaceutical industries. In situ crystallographic and spectroscopic studies reveal strong binding interactions of NO(2) to the {Zr(6)(μ(3)-O)(4)(μ(3)-OH)(4)(COO)(12)} cluster node. This study paves a circular pathway to enable the integration of nitrogen-based air pollutants into the production of fine chemicals. American Chemical Society 2022-10-05 2022-10-19 /pmc/articles/PMC9585588/ /pubmed/36198137 http://dx.doi.org/10.1021/jacs.2c07283 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Li, Jiangnan
Wang, Zi
Chen, Yinlin
Cheng, Yongqiang
Daemen, Luke L.
Tuna, Floriana
McInnes, Eric J. L.
Day, Sarah J.
Ramirez-Cuesta, Anibal J.
Schröder, Martin
Yang, Sihai
Synthesis of Nitro Compounds from Nitrogen Dioxide Captured in a Metal-Organic Framework
title Synthesis of Nitro Compounds from Nitrogen Dioxide Captured in a Metal-Organic Framework
title_full Synthesis of Nitro Compounds from Nitrogen Dioxide Captured in a Metal-Organic Framework
title_fullStr Synthesis of Nitro Compounds from Nitrogen Dioxide Captured in a Metal-Organic Framework
title_full_unstemmed Synthesis of Nitro Compounds from Nitrogen Dioxide Captured in a Metal-Organic Framework
title_short Synthesis of Nitro Compounds from Nitrogen Dioxide Captured in a Metal-Organic Framework
title_sort synthesis of nitro compounds from nitrogen dioxide captured in a metal-organic framework
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9585588/
https://www.ncbi.nlm.nih.gov/pubmed/36198137
http://dx.doi.org/10.1021/jacs.2c07283
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