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

Shaojun Xu, Xue Han, Yujie Ma, Thien D. Duong, Longfei Lin, Emma K. Gibson, Alena Sheveleva, Sarayute Chansai, Alex Walton, Duc The Ngo, Mark D. Frogley, Chiu C. Tang, Floriana Tuna, Eric J.L. McInnes, C. Richard A. Catlow, Christopher Hardacre, Sihai Yang, Martin Schröder

Research output: Contribution to journalArticlepeer-review

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. Nitrogen oxide causes significant effects on the environment and human health. Xu et al. report, to the best of their knowledge, the first example of nonthermal plasma-activated direct decomposition of NO2 over stable and efficient metal-organic framework-based catalysts at room temperature and without the use of NH3 or other reducing agents.

Original languageEnglish
Article number100349
JournalCell Reports Physical Science
Volume2
Issue number2
Early online date17 Feb 2021
DOIs
Publication statusPublished - 24 Feb 2021

Keywords

  • catalysis
  • copper
  • DRIFTs
  • EPR
  • low-temperature NO reduction
  • metal-organic framework
  • MFM-300(Al)
  • NO
  • non-thermal plasma
  • XAFS

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