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过渡金属替代的CeO2(111)表面上NO+CO反应机理的理论研究

丁戊辰 ,  李微雪

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引用本文: 丁戊辰, 李微雪. 过渡金属替代的CeO2(111)表面上NO+CO反应机理的理论研究[J]. 催化学报, 2014, 35(12): 1937-1943. doi: 10.1016/S1872-2067(14)60169-8 shu
Citation:  Wuchen Ding, Weixue Li. First-principles study of NO reduction by CO on transition metal atoms-doped CeO2(111)[J]. Chinese Journal of Catalysis, 2014, 35(12): 1937-1943. doi: 10.1016/S1872-2067(14)60169-8 shu

过渡金属替代的CeO2(111)表面上NO+CO反应机理的理论研究

    通讯作者: 李微雪
  • 基金项目:

    国家自然科学基金(21173210, 21225315) (21173210, 21225315)

    国家重点基础研究发展计划(973计划, 2013CB834603) (973计划, 2013CB834603)

    中国科学院战略性先导科技专项(XDA09030000). (XDA09030000)

摘要: 采用DFT+U方法研究了过渡金属替代的CeO2(111)表面上的NO+CO反应机理, 以探求不同过渡金属对N2选择性的影响.结果表明, 在反应过程中, 反应活性中心由过渡金属单原子与其最近邻的氧空位组成.NO在过渡金属-氧空位上发生N-O断键, 不同过渡金属上该还原步骤的难易程度不同.计算发现, 右过渡金属Rh, Pd和Pt替代的CeO2(111)表面可以与吸附物之间形成较强的吸附作用, 进而可以达到较高的N2选择性. 其主要原因是右过渡金属具有较多的d电子, 可以与吸附小分子之间形成有效的反馈键.而左过渡金属拥有较少的d电子, 难以有效抓住吸附物, 最终导致较低的N2选择性.

English

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  • 收稿日期:  2014-05-16
  • 网络出版日期:  2014-06-10
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