Plasma-Triggered CH4/NH3 Coupling Reaction for Direct Synthesis of Liquid Nitrogen-Containing Organic Chemicals.

Abstract

Nitrogen-containing organic chemicals such as amines, amides, nitriles, and hydrazones are crucial in chemical and medical industries. This paper reports a direct synthesis of N,N-dimethyl cyanamide [(CH3)2NCN] and amino acetonitrile (NH2CH2CN) through a methane/ammonia (CH4/NH3) coupling reaction triggered by dielectric barrier discharge plasma, with by-products of hydrazine, amines, and hydrazones. The influence of CH4/NH3 molar ratio, feedstock residence time, and specific energy input on the CH4/NH3 plasma coupling reaction has been investigated and discussed. Under the optimized conditions, the productivities of (CH3)2NCN and NH2CH2CN reached 0.46 and 0.82 g·L–1·h–1, respectively, with 8.83% CH4 conversion. In addition, through combining the optical emission spectra diagnosis and the reaction results, a possible CH4/NH3 plasma coupling reaction mechanism has been proposed. This paper provides a potential fine application of CH4 and NH3 in green synthesis of liquid nitrogen-containing organic chemicals, such as nitriles, amines, amides, and hydrazones.