Plasma-Catalytic Ammonia Reforming of Methane over Cu-Based Catalysts for the Production of HCN and H<sub>2</sub> at Reduced Temperature
Yanhui Yi, Xin Wang, Amin Jafarzadeh, Li Wang, Pei Liu, Bowen He, Jinhui Yan, Rui Zhang, Hantian Zhang, Xi Liu, Hongchen Guo, Erik C. Neyts, Annemie Bogaerts
Abstract
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.