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Modulation of uptake and reactivity of nitrogen dioxide in metal-organic framework materials

DOI: 10.1002/anie.202302602 DOI Help

Authors: Zi Wang (The University of Manchester) , Alena M. Sheveleva (The University of Manchester) , Daniel Lee (The University of Manchester) , Yinlin Chen (The University of Manchester) , Dinu Iuga (The University of Manchester) , W. Trent Franks (The University of Manchester) , Yujie Ma (The University of Manchester) , Jiangnan Li (The University of Manchester) , Lei Li (The University of Manchester) , Yongqiang Cheng (Oak Ridge National Laboratory) , Luke L. Daemen (Oak Ridge National Laboratory) , Sarah J. Day (Diamond Light Source) , Anibal J. Ramirez-Cuesta (Oak Ridge National Laboratory) , Bing Han (The University of Manchester) , Alexander S. Eggeman (The University of Manchester) , Eric J. L. Mcinnes (The University of Manchester) , Floriana Tuna (The University of Manchester) , Sihai Yang (The University of Manchester) , Martin Schroeder (The University of Manchester)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Angewandte Chemie International Edition

State: Published (Approved)
Published: April 2023

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.

Journal Keywords: metal-organic framework; nitrogen dioxide; reactivity modulation; conversion; spectrography

Diamond Keywords: Gas Separation

Subject Areas: Chemistry, Materials, Environment

Instruments: I11-High Resolution Powder Diffraction

Other Facilities: VISION at ORNL

Added On: 09/04/2023 10:51

Discipline Tags:

Desertification & Pollution Earth Sciences & Environment Chemistry Materials Science Metal-Organic Frameworks Metallurgy Organometallic Chemistry

Technical Tags:

Diffraction X-ray Powder Diffraction