Kinetics of NO reduction by CO over supported rhodium catalysts: Isotopic cycling experiments

Kinetics of NO reduction by CO over supported rhodium catalysts: Isotopic cycling experiments
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DOI:
10.1016/0021-9517(89)90052-3
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发表时间:
1989-02
影响因子:
7.3
通讯作者:
B. Cho;B. Shanks;J. Bailey
B. Cho;B. Shanks;J. Bailey
中科院分区:
化学1区
文献类型:
--
作者:
B. Cho;B. Shanks;J. Bailey

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在填充床反应器上,以13 CO为反应物,考察了Rh Al 2 O3和Rh CeO 2催化剂在循环进料条件和稳定进料条件下对CO还原NO反应的催化活性.结果表明,在Rh Al 2 O3催化剂上(CO+ NO)反应过程中,N2 O的生成是一个重要的中间步骤.从CeO 2载体的储氧能力出发,讨论了Rh-CeO 2催化剂在循环操作条件下比Rh-Al 2 O3催化剂活性的提高。考虑到随温度变化的速率控制步骤的性质,检查不对称循环的效果。在此基础上,提出了Rh Al 2 O3催化剂上(CO+ NO)反应的一个总体反应方案,其中N2 O作为反应中间体。
The catalytic activity of Rh Al 2 O 3 and Rh CeO 2 catalysts was investigated for the reduction of NO by CO under feed-composition cycling conditions as well as under steady feed conditions using a packed-bed reactor and an isotopic reactant, 13 CO. Results indicate that the formation of N 2 O is an important intermediate step during the (CO+ NO) reaction over Rh Al 2 O 3. The enhanced catalytic activity of Rh CeO 2 compared with Rh Al 2 O 3 under cyclic operating conditions is discussed in light of the oxygen storage capacity of ceria support. The effect of asymmetric cycling is examined in view of the nature of the rate-controlling step which changes with temperature. On the basis of our observations an overall reaction scheme is proposed for the (CO+ NO) reaction over Rh Al 2 O 3 in which N 2 O is included as a reaction intermediate.