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

DOI: 10.1016/j.xcrp.2021.100349 DOI Help

Authors: Shaojun Xu (University of Manchester; UK Catalysis Hub, Research Complex at Harwell) , Xue Han (University of Manchester) , Yujie Ma (University of Manchester) , Thien D. Duong (University of Manchester) , Longfei Lin (University of Manchester) , Emma K. Gibson (UK Catalysis Hub, Research Complex at Harwell; University of Glasgow) , Alena Sheveleva (University of Manchester) , Sarayute Chansai (University of Manchester) , Alex Walton (University of Manchester) , Duc-The Ngo (University of Manchester) , Mark D. Frogley (Diamond Light Source) , Chiu C. Tang (Diamond Light Source) , Floriana Tuna (University of Manchester) , Eric J. L. Mcinnes (University of Manchester) , C. Richard A. Catlow (UK Catalysis Hub, Research Complex at Harwell; Cardiff University; University College London) , Christopher Hardacre (University of Manchester) , Sihai Yang (University of Manchester,) , Martin Schroeder (University of Manchester)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Cell Reports Physical Science , VOL 3

State: Published (Approved)
Published: February 2021

Open Access Open Access

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.

Journal Keywords: low-temperature NOx reduction;NO2; non-thermal plasma; metal-organic framework; MFM-300(Al); DRIFTs; XAFS; EPR; catalysis; copper

Subject Areas: Chemistry, Materials, Environment

Instruments: B18-Core EXAFS , B22-Multimode InfraRed imaging And Microspectroscopy , I11-High Resolution Powder Diffraction

Added On: 18/02/2021 15:55


Discipline Tags:

Desertification & Pollution Earth Sciences & Environment Physical Chemistry Catalysis Chemistry

Technical Tags:

Diffraction Spectroscopy X-ray Powder Diffraction Infrared Spectroscopy X-ray Absorption Spectroscopy (XAS) Synchtron-based Fourier Transform Infrared Spectroscopy (SR-FTIR)