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Promotional mechanism of activity via three-dimensional ordered macroporous Cu-doped Ce–Fe mixed oxides for the CO-SCR reaction
Environmental Science: Nano ( IF 7.3 ) Pub Date : 2020-09-01 , DOI: 10.1039/d0en00696c
Hao Liu 1, 2, 3, 4, 5 , Qiuxia Liang 1, 2, 3, 4, 5 , Jiaxing Liu 1, 2, 3, 4, 5 , Xia Liu 1, 2, 3, 4, 5 , Danyang Li 1, 2, 3, 4, 5 , Shangzhi Xie 1, 2, 3, 4, 5 , Lijian Jin 1, 2, 3, 4, 5 , Lihui Dong 1, 2, 3, 4, 5 , Bin Li 1, 2, 3, 4, 5 , Yinchao Yao 1, 2, 3, 4, 5
Affiliation  

A series of doped rather than supported 3DOM Ce0.7Fe0.2M0.1O2 and bulk Ce0.7Fe0.2Cu0.1O2 catalysts were prepared for the CO-SCR reaction. The formation of the 3DOM structure not only improves the reduction performance and surface-active sites but also promotes the generation of more surface-adsorbed oxygen species. Thus, the 3DOM Ce0.7Fe0.2Cu0.1O2 catalyst shows high CO-SCR activity in the broad operating temperature window of 150–700 °C, with T50 at 150 °C and T100 at 350 °C. It also has the highest CO oxidation activity in a series of samples. Moreover, the appearance of Cu+–CO species and the fast transition between Ce4+ and Ce3+ (Cu2+ + Ce3+ ↔ Cu+ + Ce4+) are the reasons why 3DOM Ce0.7Fe0.2Cu0.1O2 has better catalytic activity than other catalysts at lower temperature. Simultaneously, the oxygen vacancies produced by the reduction of Fe3+ → Fe2+ and those adjacent to Ce3+ are more significant at higher temperatures, and are favorable for the dissociation of NO. The cause of partial deactivation of the optimal catalyst under specific reaction conditions is also discovered, which further confirms the importance of Cu+ and number of active sites. Further, the CO-SCR reaction on 3DOM Ce0.7Fe0.2Cu0.1O2 follows the mechanism of L–H and E–R at low and high temperatures, respectively.

中文翻译:

三维有序大孔掺铜铈铁混合氧化物对CO-SCR反应的促进作用机理

制备了一系列掺杂而不是负载的3DOM Ce 0.7 Fe 0.2 M 0.1 O 2和本体Ce 0.7 Fe 0.2 Cu 0.1 O 2催化剂用于CO-SCR反应。3DOM结构的形成不仅提高了还原性能和表面活性位,而且促进了更多表面吸附氧的产生。因此,3DOM Ce 0.7 Fe 0.2 Cu 0.1 O 2催化剂在150-700°C的宽工作温度范围内具有高的CO-SCR活性,T 50在150°C和T 100在350°C下。它还在一系列样品中具有最高的CO氧化活性。此外,Cu + –CO物种的出现以及Ce 4+和Ce 3+(Cu 2+ + Ce 3+ ↔Cu + + Ce 4+)之间的快速转变是3DOM Ce 0.7 Fe 0.2 Cu 0.1 O的原因。2在较低温度下比其他催化剂具有更好的催化活性。同时,还原Fe 3+ →Fe 2+以及与Ce 3+相邻的氧空位在较高温度下它们更重要,并且对于NO的离解是有利的。还发现了在特定反应条件下最佳催化剂部分失活的原因,这进一步证实了Cu +的重要性和活性位点的数量。此外,在3DOM Ce 0.7 Fe 0.2 Cu 0.1 O 2上的CO-SCR反应分别遵循L–H和E–R在低温和高温下的机理。
更新日期:2020-10-17
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