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Catalytic decomposition of HCN on copper manganese oxide at low temperatures: performance and mechanism
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2018-04-10
Yingjie Li, Huai Yang, Yuechao Zhang, Jing Hu, Jianhong Huang, Ping Ning, Senlin Tian

The Development of innovative treatment technology for HCN at low temperatures is vital for the control of HCN pollution. Here, a copper manganese oxide (Cu-Mn-O) catalyst was prepared for the decomposition of HCN at temperatures from 80 to 200 °C. The results showed that the Cu-Mn-O catalyst exhibited excellent catalytic performance for HCN conversion. X-ray photoelectron spectroscopy analysis revealed that Mn3+ manifested highly catalytic activity and was largely responsible for HCN decomposition. The N-contained products of HCN contained NH3, NO/NO2, N2O, and N2, thereby suggesting the concurrent catalytic oxidation and hydrolysis during HCN decomposition on the catalyst. The catalytic oxidation mechanism characterized by in situ diffuse reflectance infrared Fourier transform manifested that four N-contained intermediates (i.e., -CN, -NH2, =NH and -NCO) were produced; subsequent the oxidation of these intermediates resulted in the formation of final product and/or oxidative species NO+. The reaction of NO+ with the N-contained intermediates also generated the final conversion products. Catalytic intermediate formamide plays a critical role in the hydrolysis of HCN, and its hydrolysis leads to the formation of NH3. Multiple cycle experiments demonstrate the long-term stability of the Cu-Mn-O catalyst. These results indicate that catalytic decomposition of HCN based on the Cu-Mn-O catalyst at low temperatures may be an efficient approach for the treatment of tail gases containing HCN.



中文翻译:

氰化铜锰氧化物上HCN在低温下的催化分解:性能与机理

低温HCN的创新处理技术的发展对于控制HCN污染至关重要。此处,制备了铜锰氧化物(Cu-Mn-O)催化剂,用于在80至200℃的温度下分解HCN。结果表明,Cu-Mn-O催化剂对HCN的转化表现出优异的催化性能。X射线光电子能谱分析表明,Mn 3+表现出很高的催化活性,并在很大程度上负责HCN的分解。HCN的N含产物包含NH 3,NO / NO 2,N 2 O和N 2,因此表明在催化剂上HCN分解过程中同时发生催化氧化和水解。以原位漫反射红外傅里叶变换为特征的催化氧化机理表明,生成了四种含氮中间体(即-CN,-NH 2,= NH和-NCO)。随后这些中间体的氧化导致最终产物和/或氧化性物种NO +的形成。NO +与含N的中间体的反应也产生了最终的转化产物。催化中间体甲酰胺在HCN的水解中起关键作用,其水解导致NH 3的形成。多循环实验证明了Cu-Mn-O催化剂的长期稳定性。这些结果表明,在低温下基于Cu-Mn-O催化剂的HCN催化分解可能是处理含HCN尾气的有效方法。

更新日期:2018-04-11
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