Enhanced activity and sulfur resistance for soot combustion on three-dimensionally ordered macroporous-mesoporous MnxCe1-xO delta/SiO2 catalysts
Enhanced activity and sulfur resistance for soot combustion on three-dimensionally ordered macroporous-mesoporous MnxCe1-xO delta/SiO2 catalysts
复制标题
三维有序大孔-介孔MnxCe1-xO delta/SiO2催化剂的烟灰燃烧活性和抗硫性能增强
DOI：
10.1016/j.apcatb.2019.04.097
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发表时间：
2019
期刊：
影响因子：
--
通讯作者：
Liu Jian
中科院分区：
文献类型：
--
作者：
Yu Xuehua;Wang Lanyi;Chen Maozhong;Fan Xiaoqiang;Zhao Zhen;Cheng Kai;Chen Yongsheng;Sojka Zbigniew;Wei Yuechang;Liu Jian
设计了一系列不同Mn_（0.5）Ce_（0.5）O_δ负载量和不同x值的Mn_xCe_（1-x）O_δ/3DOM-mSiO_2催化剂，并通过一种非常简单的方法成功地制备了这些催化剂。所制备的催化剂具有三维有序大孔（3DOM）结构和有序介孔结构，对碳烟燃烧具有较高的催化活性和良好的稳定性。结果表明，所制备的催化剂具有较好的催化性能，这主要是由于Mn和Ce在介孔结构中促进了碳烟的传输，以及Mn和Ce对介孔结构中气体分子（NO和O2）的协同活化作用。此外，对制备的催化剂进行了耐硫、耐水性能测试，并对耐硫、耐水的原因进行了分析。根据表征结果和DFT计算，提出了碳烟燃烧的可能机理。更重要的是，这项工作展示了大固体颗粒和小气体分子之间反应的高效催化剂的合理设计和容易制备。
A series of MnxCe1-xOδ/3DOM-m SiO2catalysts with different Mn0.5Ce0.5Oδloadings and different x values were designed and successfully prepared by a very simple method. The as-prepared catalysts, which contain three-dimensionally ordered macroporous (3DOM) structure embedded with ordered mesoporous structure, exhibit high catalytic activity and good stability for soot combustion. The good catalytic performances of as-prepared catalysts are owing to facilitated soot transport through the macroporous structure and synergistic effect between Mn and Ce for the activation of gas molecules (NO and O2) within the mesoporous structure. In addition, the sulfur and water tolerance of as-prepared catalysts were tested and the reasons for sulfur and water tolerance also well illustrated. The probable soot combustion mechanisms are proposed based on the characterization results and DFT calculation. More importantly, this work demonstrates the rational design and facile preparation of highly efficient catalysts for reactions between large solid particles and small gas molecules.