Pt/TS-1 Catalyst Promoted C-N Coupling Reaction in CH4-NH3 Plasma for HCN Synthesis at Low Temperature
Pt/TS-1 Catalyst Promoted C-N Coupling Reaction in CH4-NH3 Plasma for HCN Synthesis at Low Temperature
复制标题
Pt/TS-1 催化剂促进 CH4-NH3 等离子体中的 C-N 偶联反应用于低温合成 HCN
DOI：
10.1021/acscatal.8b02950
复制
发表时间：
2018-11-01
期刊：
影响因子：
12.9
通讯作者：
Guo, Hongchen
中科院分区：
文献类型：
--
作者：
Guo, Zhifang;Yi, Yanhui;Guo, Hongchen
氢氰酸是化学工业中一种重要的合成材料。目前，生产HCN的工业方法主要包括安德卢梭法和BMA法，其必须在超过1000 ℃的温度下操作。本文提出了一种在低温（400 ℃）下，以Pt/TS-1为催化剂，在CH 4/NH3等离子体中通过C-N偶联反应合成HCN的方法。在优化的反应条件下（CH 4/NH3 = 1：2，GHSV：2425 s（-1），放电长度：3 cm，反应温度：400 ℃，Pt/TS-1 +等离子体），HCN选择性达到80.9%，CH 4转化率为25.9%。在反应过程中，低温等离子体起到了活化CH 4和NH3生成自由基物种（CHx和NHy）的作用，而Pt/TS-1催化剂则促进了自由基物种的C-N偶联反应生成HCN。
Hydrocyanic acid is an important synthetic material in chemical industry. Currently, the industrial methods of producing HCN mainly include the Andrussow and BMA processes, which are necessarily operated at temperatures of more than 1000 degrees C. This paper proposes a method to synthesize HCN at low temperature (400 degrees C) through a C-N coupling reaction in CH4/NH3 nonthermal plasma with the assistance of Pt/TS-1 catalyst. Under the optimized reaction conditions (CH4/NH3 = 1:2, GHSV: 2425 s(-1), discharge length: 3 cm, reaction temperature: 400 degrees C, Pt/TS-1 + plasma), 80.9% HCN selectivity was achieved with 25.9% CH4 conversion. During the reaction process, the nonthermal plasma played a role of activating CH4 and NH3 into radical species (CHx and NHy), while the Pt/TS-1 catalyst promoted the C-N coupling reaction of the radical species to produce HCN.