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

Xu, Shaojun, Han, Xue, Ma, Yujie, Duong, Thien D., Lin, Longfei, Gibson, Emma K., Sheveleva, Alena, Chansai, Sarayute, Walton, Alex, Ngo, Duc-The, Frogley, Mark D., Tang, Chiu C., Tuna, Floriana, McInnes, Eric J.L., Catlow, C. Richard A., Hardacre, Christopher, Yang, Sihai and Schröder, Martin 2021. Catalytic decomposition of NO2 over a copper-decorated metal-organic framework by non-thermal plasma. Cell Reports Physical Science 2 (2) , 100349. 10.1016/j.xcrp.2021.100349

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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.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI) Advanced Research Computing @ Cardiff (ARCCA)
Additional Information:	This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
Publisher:	Elsevier
ISSN:	2666-3864
Funders:	EPSRC and Royal Society
Date of First Compliant Deposit:	10 March 2021
Date of Acceptance:	27 January 2021
Last Modified:	05 May 2023 23:45
URI:	https://orca.cardiff.ac.uk/id/eprint/139448

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