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Catalytic decomposition of NO2 over a copper-decorated metal–organic framework by non-thermal plasma

Xu, S; Han, X; Ma, Y; Duong, TD; Lin, L; Gibson, EK; Sheveleva, A; ... Schröder, M; + view all (2021) Catalytic decomposition of NO2 over a copper-decorated metal–organic framework by non-thermal plasma. Cell Reports Physical Science , 2 (2) , Article 100349. 10.1016/j.xcrp.2021.100349. Green open access

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Abstract

Efficient catalytic conversion of NO2 to non-harmful species remains an important target for research. State-of-the-art deNOx processes are based upon ammonia (NH3)-assisted selective catalytic reduction (NH3-SCR) over Cu-exchanged zeolites at elevated temperatures. Here, we describe a highly efficient non-thermal plasma (NTP) deNOx process catalyzed by a Cu-embedded metal-organic framework, Cu/MFM-300(Al), at room temperature. Under NTP activation at 25°C, Cu/MFM-300(Al) enables direct decomposition of NO2 into N2, NO, N2O, and O2 without the use of NH3 or other reducing agents. NO2 conversion of 96% with a N2 selectivity of 82% at a turnover frequency of 2.9 h−1 is achieved, comparable to leading NH3-SCR catalysts that use NH3 operating at 250°C–550°C. The mechanism for the rate-determining step (NO→N2) is elucidated by in operando diffuse reflectance infrared Fourier transform spectroscopy, and electron paramagnetic resonance spectroscopy confirms the formation of Cu2+⋯NO nitrosylic adducts on Cu/MFM-300(Al), which facilitates NO dissociation and results in the notable N2 selectivity.

Type: Article
Title: Catalytic decomposition of NO2 over a copper-decorated metal–organic framework by non-thermal plasma
Open access status: An open access version is available from UCL Discovery
DOI: 10.1016/j.xcrp.2021.100349
Publisher version: http://doi.org/10.1016/j.xcrp.2021.100349
Language: English
Additional information: This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10123108
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