MODULATION OF UPTAKE AND REACTIVITY OF NITROGEN DIOXIDE IN METAL‐ORGANIC FRAMEWORK MATERIALS

Zi Wang; Alena M. Sheveleva; Daniel Lee; Yinlin Chen; Dinu Iuga; W. Trent Franks; Yujie Ma; Jiangnan Li; Lei Li; Yongqiang Cheng; Luke L. Daemen; Sarah J. Days; Anibal J. Ramirez-Cuesta; Bing Han; Alexander S. Eggeman; Eric J. L. Mcinnes; Floriana Tuna; Sihai Yang; Martin Schröder

doi:10.1002/anie.202302602

MODULATION OF UPTAKE AND REACTIVITY OF NITROGEN DIOXIDE IN METAL‐ORGANIC FRAMEWORK MATERIALS

Zi Wang, Alena M. Sheveleva, Daniel Lee, Yinlin Chen, Dinu Iuga, W. Trent Franks, Yujie Ma, Jiangnan Li, Lei Li, Yongqiang Cheng, Luke L. Daemen, Sarah J. Days, Anibal J. Ramirez-Cuesta, Bing Han, Alexander S. Eggeman, Eric J. L. Mcinnes, Floriana Tuna, Sihai Yang, Martin Schröder

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Abstract

We report the modulation of reactivity of nitrogen dioxide (NO2) in a charged metal-organic framework (MOF) material, MFM-305-CH3 in which unbound N-centres are methylated and the cationic charge counter-balanced by Cl− ions in the pores. Uptake of NO2 into MFM-305-CH3 leads to reaction between NO2 and Cl– to give nitrosyl chloride (NOCl) and NO3− anions. A high dynamic uptake of 6.58 mmol g−1 at 298 K is observed for MFM-305-CH3 as measured using a flow of 500 ppm NO2 in He. In contrast, the analogous neutral material, MFM-305, shows a much lower uptake of 2.38 mmol g−1. The binding domains and reactivity of adsorbed NO2 molecules within MFM-305-CH3 and MFM-305 have been probed using in situ synchrotron X-ray diffraction, inelastic neutron scattering and by electron paramagnetic resonance, high-field solid-state nuclear magnetic resonance and UV-vis spectroscopies. The design of charged porous sorbents provides a new platform to control the reactivity of corrosive air pollutants.

Original language	English
Journal	Angewandte Chemie International Edition
Early online date	7 Apr 2023
DOIs	https://doi.org/10.1002/anie.202302602
Publication status	E-pub ahead of print - 7 Apr 2023

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Wang, Z., Sheveleva, A. M., Lee, D., Chen, Y., Iuga, D., Franks, W. T., Ma, Y., Li, J., Li, L., Cheng, Y., Daemen, L. L., Days, S. J., Ramirez-Cuesta, A. J., Han, B., Eggeman, A. S., Mcinnes, E. J. L., Tuna, F., Yang, S., & Schröder, M. (2023). MODULATION OF UPTAKE AND REACTIVITY OF NITROGEN DIOXIDE IN METAL‐ORGANIC FRAMEWORK MATERIALS. Angewandte Chemie International Edition. Advance online publication. https://doi.org/10.1002/anie.202302602

@article{7dadf89df3974c1d9d3d8ffc381a1871,

title = "MODULATION OF UPTAKE AND REACTIVITY OF NITROGEN DIOXIDE IN METAL‐ORGANIC FRAMEWORK MATERIALS",

abstract = "We report the modulation of reactivity of nitrogen dioxide (NO2) in a charged metal-organic framework (MOF) material, MFM-305-CH3 in which unbound N-centres are methylated and the cationic charge counter-balanced by Cl− ions in the pores. Uptake of NO2 into MFM-305-CH3 leads to reaction between NO2 and Cl– to give nitrosyl chloride (NOCl) and NO3− anions. A high dynamic uptake of 6.58 mmol g−1 at 298 K is observed for MFM-305-CH3 as measured using a flow of 500 ppm NO2 in He. In contrast, the analogous neutral material, MFM-305, shows a much lower uptake of 2.38 mmol g−1. The binding domains and reactivity of adsorbed NO2 molecules within MFM-305-CH3 and MFM-305 have been probed using in situ synchrotron X-ray diffraction, inelastic neutron scattering and by electron paramagnetic resonance, high-field solid-state nuclear magnetic resonance and UV-vis spectroscopies. The design of charged porous sorbents provides a new platform to control the reactivity of corrosive air pollutants.",

author = "Zi Wang and Sheveleva, {Alena M.} and Daniel Lee and Yinlin Chen and Dinu Iuga and Franks, {W. Trent} and Yujie Ma and Jiangnan Li and Lei Li and Yongqiang Cheng and Daemen, {Luke L.} and Days, {Sarah J.} and Ramirez-Cuesta, {Anibal J.} and Bing Han and Eggeman, {Alexander S.} and Mcinnes, {Eric J. L.} and Floriana Tuna and Sihai Yang and Martin Schr{\"o}der",

year = "2023",

month = apr,

day = "7",

doi = "10.1002/anie.202302602",

language = "English",

journal = "Angewandte Chemie International Edition",

issn = "1433-7851",

publisher = "John Wiley & Sons Ltd",

}

Wang, Z, Sheveleva, AM, Lee, D, Chen, Y, Iuga, D, Franks, WT, Ma, Y, Li, J, Li, L, Cheng, Y, Daemen, LL, Days, SJ, Ramirez-Cuesta, AJ, Han, B, Eggeman, AS , Mcinnes, EJL , Tuna, F, Yang, S & Schröder, M 2023, 'MODULATION OF UPTAKE AND REACTIVITY OF NITROGEN DIOXIDE IN METAL‐ORGANIC FRAMEWORK MATERIALS', Angewandte Chemie International Edition. https://doi.org/10.1002/anie.202302602

TY - JOUR

T1 - MODULATION OF UPTAKE AND REACTIVITY OF NITROGEN DIOXIDE IN METAL‐ORGANIC FRAMEWORK MATERIALS

AU - Wang, Zi

AU - Sheveleva, Alena M.

AU - Lee, Daniel

AU - Chen, Yinlin

AU - Iuga, Dinu

AU - Franks, W. Trent

AU - Ma, Yujie

AU - Li, Jiangnan

AU - Li, Lei

AU - Cheng, Yongqiang

AU - Daemen, Luke L.

AU - Days, Sarah J.

AU - Ramirez-Cuesta, Anibal J.

AU - Han, Bing

AU - Eggeman, Alexander S.

AU - Mcinnes, Eric J. L.

AU - Tuna, Floriana

AU - Yang, Sihai

AU - Schröder, Martin

PY - 2023/4/7

Y1 - 2023/4/7

N2 - We report the modulation of reactivity of nitrogen dioxide (NO2) in a charged metal-organic framework (MOF) material, MFM-305-CH3 in which unbound N-centres are methylated and the cationic charge counter-balanced by Cl− ions in the pores. Uptake of NO2 into MFM-305-CH3 leads to reaction between NO2 and Cl– to give nitrosyl chloride (NOCl) and NO3− anions. A high dynamic uptake of 6.58 mmol g−1 at 298 K is observed for MFM-305-CH3 as measured using a flow of 500 ppm NO2 in He. In contrast, the analogous neutral material, MFM-305, shows a much lower uptake of 2.38 mmol g−1. The binding domains and reactivity of adsorbed NO2 molecules within MFM-305-CH3 and MFM-305 have been probed using in situ synchrotron X-ray diffraction, inelastic neutron scattering and by electron paramagnetic resonance, high-field solid-state nuclear magnetic resonance and UV-vis spectroscopies. The design of charged porous sorbents provides a new platform to control the reactivity of corrosive air pollutants.

AB - We report the modulation of reactivity of nitrogen dioxide (NO2) in a charged metal-organic framework (MOF) material, MFM-305-CH3 in which unbound N-centres are methylated and the cationic charge counter-balanced by Cl− ions in the pores. Uptake of NO2 into MFM-305-CH3 leads to reaction between NO2 and Cl– to give nitrosyl chloride (NOCl) and NO3− anions. A high dynamic uptake of 6.58 mmol g−1 at 298 K is observed for MFM-305-CH3 as measured using a flow of 500 ppm NO2 in He. In contrast, the analogous neutral material, MFM-305, shows a much lower uptake of 2.38 mmol g−1. The binding domains and reactivity of adsorbed NO2 molecules within MFM-305-CH3 and MFM-305 have been probed using in situ synchrotron X-ray diffraction, inelastic neutron scattering and by electron paramagnetic resonance, high-field solid-state nuclear magnetic resonance and UV-vis spectroscopies. The design of charged porous sorbents provides a new platform to control the reactivity of corrosive air pollutants.

U2 - 10.1002/anie.202302602

DO - 10.1002/anie.202302602

M3 - Article

SN - 1433-7851

JO - Angewandte Chemie International Edition

JF - Angewandte Chemie International Edition

ER -

MODULATION OF UPTAKE AND REACTIVITY OF NITROGEN DIOXIDE IN METAL‐ORGANIC FRAMEWORK MATERIALS

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