期刊
JOURNAL OF CATALYSIS
卷 208, 期 1, 页码 180-186出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1006/jcat.2002.3571
关键词
ammonia synthesis; microkinetic analysis; dinitrogen adsorption; promotion; nitride catalyst
The kinetics of ammonia synthesis and N-2 dissociation over cesium-promoted Co3Mo3N are studied. The results support recent DFT calculations and explain why Co3Mo3N shows a higher ammonia synthesis activity than either constituting metal. The ammonia synthesis activity of cesium-promoted Co3Mo3N is reported for a series of conditions, with H-2 : N-2 ratios of both 3 : 1 and 1 : 1, total pressures of 50, 25, and 10 bar, and temperatures from 593 to 713 K. Isothermal N2 adsorption experiments were carried out and the results were well described by a simple model. The total number of surface sites on the catalyst capable of binding nitrogen was found to be approximately 30 mumol/g of catalyst. When only 1% of these surface sites is active for N-2 dissociation, the initial sticking coefficient, s(0), of dinitrogen on the active sites was found to be s(0) = 0.1727 (.) exp((-42.8 +/- 5 kJ/mol)/RT). This result was used as input to a microkinetic model for ammonia synthesis where it was assumed that N* and H* are the only surface intermediates. In this way it was possible to obtain a good fit to the ammonia synthesis activity data with the nitrogen-binding energy as the only adjustable parameter. (C) 2002 Elsevier Science (USA).
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据