Publisher: Elsevier BV

Issue: 2

License: [{"URL"=>"https://www.elsevier.com/tdm/userlicense/1.0/", "start"=>{"date-parts"=>[[2021, 2, 1]], "date-time"=>"2021-02-01T00:00:00Z", "timestamp"=>1612137600000}, "delay-in-days"=>0, "content-version"=>"tdm"}, {"URL"=>"http://creativecommons.org/licenses/by/4.0/", "start"=>{"date-parts"=>[[2021, 1, 28]], "date-time"=>"2021-01-28T00:00:00Z", "timestamp"=>1611792000000}, "delay-in-days"=>0, "content-version"=>"vor"}]

Publication date(s): 2021/02 (online)

Pages: 100349

Volume: 2 Issue: 2

Journal: Cell Reports Physical Science

Link: [{"URL"=>"https://api.elsevier.com/content/article/PII:S2666386421000345?httpAccept=text/xml", "content-type"=>"text/xml", "content-version"=>"vor", "intended-application"=>"text-mining"}, {"URL"=>"https://api.elsevier.com/content/article/PII:S2666386421000345?httpAccept=text/plain", "content-type"=>"text/plain", "content-version"=>"vor", "intended-application"=>"text-mining"}]

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.