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

Yanhui Yi; Rui Zhang; Li Wang; Jinhui Yan; Jialiang Zhang; Hongchen Guo

doi:10.1021/acsomega.7b01060

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

ACS Omega. 2017 Dec 27;2(12):9199-9210. doi: 10.1021/acsomega.7b01060. eCollection 2017 Dec 31.

Authors

Yanhui Yi¹, Rui Zhang¹, Li Wang¹, Jinhui Yan¹, Jialiang Zhang¹, Hongchen Guo¹

Affiliation

¹ State Key Laboratory of Fine Chemicals, School of Chemical Engineering, and School of Physics and Optoelectronic Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China.

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.