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Plasma-catalytic ammonia reforming of methane over Cu-based catalysts for the production of HCN and H2 at reduced temperature

Tijdschriftbijdrage - Tijdschriftartikel

Industrial production of HCN from NH3 and CH4 not only uses precious Pt or Pt−Rh catalysts but also requires extremely high temperatures (∼1600 K). From an energetic, operational, and safety perspective, a drastic decrease in temperature is highly desirable. Here, we report ammonia reforming of methane for the production of HCN and H2 at 673 K by the combination of CH4/NH3 plasma and a supported Cu/silicalite-1 catalyst. 30% CH4 conversion has been achieved with 79% HCN selectivity. Catalyst characterization and plasma diagnostics reveal that the excellent reaction performance is attributed to metallic Cu active sites. In addition, we propose a possible reaction pathway, viz. E-R reactions with N, NH, NH2, and CH radicals produced in the plasma, for the production of HCN, based on density functional theory calculations. Importantly, the Cu/silicalite-1 catalyst costs less than 5% of the commercial Pt mesh catalyst.
Tijdschrift: ACS catalysis
ISSN: 2155-5435
Volume: 11
Pagina's: 1765 - 1773
Jaar van publicatie:2021
Trefwoorden:A1 Journal article
Toegankelijkheid:Open