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A new dynamic N2O reduction system based on Rh/ceria–zirconia: from mechanistic insight towards a practical application
Catalysis Science & Technology ( IF 5 ) Pub Date : 2020-11-13 , DOI: 10.1039/d0cy02035d
Yixiao Wang 1, 2, 3, 4, 5 , Jorrit Postuma de Boer 1, 2, 3, 4, 5 , Michiel Makkee 1, 2, 3, 4, 5
Affiliation  

Simultaneous reduction of N2O in the presence of co-existing oxidants, especially NO, from industrial plants, is a challenging task. This study explores the applications of a hydrocarbon reduced Rh/Zr stabilized La doped ceria (Rh/CLZ) catalyst in N2O abatement from oxidant rich industrial exhaust streams e.g. NO, CO2, and O2. The reaction mechanism was studied by the temporal analysis of products. The obtained results revealed that hydrocarbon pretreatment led to the creation of ceria oxygen vacancies and the formation of carbon deposits on the Rh/CLZ catalyst surface. These ceria oxygen vacancies are the active sites for the selective reduction of N2O into N2, while the dissociated O atoms from N2O fill the ceria oxygen vacancies. The oxidation of the deposited carbon via the lattice ceria oxygen generates new ceria oxygen vacancies, thereby extending the catalytic cycle. The reduction of N2O over C3H6 reduced Rh/CLZ is a process combining oxygen vacancy healing and deposited carbon oxidation. The results obtained from fixed-bed reactor experiments demonstrated that the hydrocarbon reduced Rh/CLZ catalyst provided a unique and extraordinary N2O abatement performance in the presence of co-existing competing oxidants (reactivity order: N2O ∼ NO > O2 > CO2 ∼ H2O).

中文翻译:

基于Rh /二氧化铈-氧化锆的新型动态N2O还原系统:从机械原理到实际应用

在共存的氧化剂(尤其是来自工厂的氧化剂)存在下同时还原N 2 O是一项艰巨的任务。这项研究探索了烃还原的Rh / Zr稳定的La掺杂的二氧化铈(Rh / CLZ)催化剂在减少富含氧化剂的工业废气,例如NO,CO 2和O 2中的N 2 O中的应用。通过产物的时间分析研究了反应机理。所得结果表明,烃预处理导致二氧化铈氧空位的产生并在Rh / CLZ催化剂表面上形成碳沉积物。这些二氧化铈氧空位是将N 2 O选择性还原成N 2的活性位点,而从N 2 O中解离的O原子填充了二氧化铈的氧空位。经由晶格二氧化铈氧对沉积的碳的氧化产生新的二氧化铈氧空位,从而延长催化循环。N 2 O相对于C 3 H 6还原的Rh / CLZ的还原是将氧空位愈合和沉积的碳氧化结合在一起的过程。从固定床反应器实验获得的结果表明,在存在共存竞争性氧化剂的情况下,碳氢化合物还原的Rh / CLZ催化剂可提供独特而卓越的N 2 O减排性能(反应顺序:N 2 O〜NO> O 2 > CO 2 - H2 O)。
更新日期:2020-11-25
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