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MeO/CeO（Me = Fe、Co、Ni）催化剂上氧交换及NO分解反应的动力学

Kinetics of Oxygen Exchange and NO Decomposition Reaction over MeO/CeO (Me = Fe, Co, Ni) Catalysts.

作者信息

Sadovskaya Ekaterina, Pinaeva Larisa, Skazka Valerii, Prosvirin Igor

机构信息

Boreskov Institute of Catalysis SB RAS, 5, Lavrentiev Ave., 630090 Novosibirsk, Russia.

Department of Mathematics and Mechanics, Novosibirsk State University, 2, Pirogov Str., 630090 Novosibirsk, Russia.

出版信息

Materials (Basel). 2023 Jan 18;16(3):929. doi: 10.3390/ma16030929.

DOI:10.3390/ma16030929
PMID:36769936
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9918102/
Abstract

MeO/CeO (Me = Fe, Co, Ni) samples were tested in an O temperature-programmed isotope exchange and NO decomposition (deNO). A decrease in the rate of deNO in the presence of oxygen evidences the competitive adsorption of NO and O on the same sites. A study of isotope oxygen exchange revealed dissociative oxygen adsorption with the subsequent formation of surface oxygen species. The same species, more probably, result from NO adsorption and the following N evolution to the gas phase. We supposed the same mechanism of O formation from surface oxygen species in both reactions, including the stages responsible for its mobility. A detailed analysis of the kinetics of isotope exchange has been performed, and the rates of one-atom () and two-atom () types of exchange were evaluated. The rate of the stage characterizing the mobility of surface oxygen was calculated, supposing the same two-step mechanism was relevant for both types of exchange. The effect of oxygen mobility on the kinetics of deNO was estimated. An analysis of the possible pathways of isotope transfer from MeO to CeO showed that direct oxygen exchange on the Me-Ce interface makes a valuable contribution to the rate of this reaction. The principal role of the Me-Ce interface in deNO was confirmed with independent experiments on FeO/CeO samples with a different iron content.

摘要

对MeO/CeO（Me = Fe、Co、Ni）样品进行了氧程序升温同位素交换和NO分解（脱硝）测试。在有氧存在的情况下脱硝速率降低，这证明了NO和O在相同位点上的竞争性吸附。同位素氧交换研究表明存在解离性氧吸附，随后形成表面氧物种。同样的物种很可能是由NO吸附以及随后N向气相逸出产生的。我们推测在两个反应中从表面氧物种形成O的机制相同，包括其迁移的相关阶段。已对同位素交换动力学进行了详细分析，并评估了单原子（）和双原子（）类型交换的速率。假设相同的两步机制适用于两种类型的交换，计算了表征表面氧迁移的阶段速率。评估了氧迁移对脱硝动力学的影响。对从MeO到CeO的同位素转移可能途径的分析表明，Me-Ce界面上的直接氧交换对该反应速率有重要贡献。通过对不同铁含量的FeO/CeO样品进行独立实验，证实了Me-Ce界面在脱硝中的主要作用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/0f0472f1e2df/materials-16-00929-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/9e32c4e0b890/materials-16-00929-g0A1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/871a9d96801c/materials-16-00929-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/f26a6a80d443/materials-16-00929-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/2890e9fc626b/materials-16-00929-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/ad6f94883e08/materials-16-00929-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/a43796dd21ea/materials-16-00929-sch002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/dd1766eef976/materials-16-00929-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/ccbcfaf2b02f/materials-16-00929-sch003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/a27bf42ebfa8/materials-16-00929-sch004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/0f0472f1e2df/materials-16-00929-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/9e32c4e0b890/materials-16-00929-g0A1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/871a9d96801c/materials-16-00929-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/f26a6a80d443/materials-16-00929-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/2890e9fc626b/materials-16-00929-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/ad6f94883e08/materials-16-00929-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/a43796dd21ea/materials-16-00929-sch002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/dd1766eef976/materials-16-00929-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/ccbcfaf2b02f/materials-16-00929-sch003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/a27bf42ebfa8/materials-16-00929-sch004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6208/9918102/0f0472f1e2df/materials-16-00929-g005.jpg

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