Pt/TS-1 Catalyst Promoted C-N Coupling Reaction in CH4-NH3 Plasma for HCN Synthesis at Low Temperature

被引:27
作者
Guo, Zhifang [1 ]
Yi, Yanhui [1 ]
Wang, Li [2 ]
Yang, Jinhui [1 ]
Guo, Hongchen [1 ]
机构
[1] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
[2] Dalian Maritime Univ, Coll Environm Sci & Engn, Dalian 116026, Liaoning, Peoples R China
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
plasma catalysis; C-N coupling reaction; platinum catalyst; HCN synthesis; synergistic effect; HYDROGEN-CYANIDE; ATMOSPHERIC-PRESSURE; ROOM-TEMPERATURE; METHANE; AMMONIA; GAS; ACTIVATION; ATOMS;
D O I
10.1021/acscatal.8b02950
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:10219 / +
页数:11
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