CeO2纳米层对多层载体x-CeO2/3DOM Al2O3负载纳米Au催化剂催化柴油炭烟燃烧活性的影响

doi:10.1016/S1872-2067(17)62798-0

催化学报 ›› 2017, Vol. 38 ›› Issue (9): 1629-1641.DOI: 10.1016/S1872-2067(17)62798-0

• 论文 • 上一篇

CeO₂纳米层对多层载体x-CeO₂/3DOM Al₂O₃负载纳米Au催化剂催化柴油炭烟燃烧活性的影响

靳保芳^a, 韦岳长^a, 赵震^a,b, 刘坚^a, 李亚钊^a, 李人杰^a, 段爱军^a, 姜桂元^a

a 中国石油大学(北京)重质油国家重点实验室, 北京 102249;
b 沈阳师范大学能源与环境催化研究所, 辽宁沈阳 110034

收稿日期:2016-11-29 修回日期:2017-01-07 出版日期:2017-09-18 发布日期:2017-09-06
通讯作者: 赵震, 韦岳长
基金资助:
国家高技术研究发展计划（863计划，2015AA034603）；国家自然科学基金（21477146，21673142，21303263）；北京市科技新星计划（Z141109001814072）；高等学校博士学科点专项科研基金（20130007120011）；中国石油大学（北京）科学基金（YJRC-2013-13；2462013BJRC003）.

Three-dimensionally ordered macroporous CeO₂/Al₂O₃-supported Au nanoparticle catalysts:Effects of CeO₂ nanolayers on catalytic activity in soot oxidation

Baofang Jin^a, Yuechang Wei^a, Zhen Zhao^a,b, Jian Liu^a, Yazhao Li^a, Renjie Li^a, Aijun Duan^a, Guiyuan Jiang^a

a State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China;
b Institute of Catalysis for Energy and Environment, Shenyang Normal University, Shenyang 110034, Liaoning, China

Received:2016-11-29 Revised:2017-01-07 Online:2017-09-18 Published:2017-09-06
Contact: 10.1016/S1872-2067(17)62798-0
Supported by:
This work was supported by the National High Technology Research and Development Program of China (863 Program,2015AA034603),the National Natural Science Foundation of China (21477146,21673142 and 21303263),the Beijing Nova Program (Z141109001814072),the Special-ized Research Fund for the Doctoral Program of Higher Education (20130007120011),and the Science Foundation of China University of Petroleum-Beijing (YJRC-2013-13,2462013BJRC003).

摘要/Abstract

摘要：

与汽油车相比，柴油车具有CO₂排放低、寿命长和经济性好等优点，所以近年来受到广泛关注并被大量使用.但是，柴油车在使用过程中会产生大量炭烟颗粒物（PM），对大气环境和人类健康造成很大威胁.因此，开展这方面的基础研究具有重要的科学意义及环境保护意义.催化柴油炭烟燃烧反应是一个气-固-固多相深度氧化反应，由于PM的粒径远大于传统催化剂，导致PM不能进入催化剂孔道内部，造成催化剂活性比表面积利用率较低.设计并制备大孔径的三维有序大孔结构（3DOM）的催化剂，能够减小反应扩散阻力，增加催化剂与炭烟颗粒物的有效接触，加快反应进行.另外，可以通过在3DOM氧化物表面担载其它活性组分，提高催化剂的氧化还原性能，进而提高其活性.
CeO₂有很好的储放氧性能，在柴油车尾气净化催化剂中较为常见，但是单一的CeO₂热稳定性较差，高温下容易烧结，使得比表面积减小，并且失去储氧能力，造成催化剂失活.文献中较常见的解决办法是在CeO₂中掺杂其它阳离子，如Zr⁴⁺，Pr³⁺，Al³⁺，La³⁺及Y³⁺等离子，以提高CeO₂的抗高温烧结能力.此外，研究报道的催化剂对催化柴油炭烟颗粒物燃烧的峰值温度已经远低于炭烟颗粒物的自燃温度，但是对颗粒物的起燃温度仍普遍较高.我们前期研究结果表明，担载纳米Au颗粒催化剂能够显著降低炭烟燃烧的起燃温度.
本文采用胶体晶体模板法制备了3DOM Al₂O₃载体，利用微孔膜-氨沉淀法担载不同量的活性组分CeO₂，制备出一种负载型x-CeO₂/3DOM Al₂O₃催化剂，它既可减少稀土元素用量，降低成本，又因为Al₂O₃的机械强度较高，还能保证催化剂的机械强度足够好.为了进一步降低催化剂催化炭烟燃烧的起燃温度，利用还原沉积法在多层载体x-CeO₂/3DOM Al₂O₃上负载纳米Au催化剂，制备出不同厚度的CeO₂纳米层负载Au催化剂（Au/x-CeO₂/3DOM Al₂O₃）.利用X射线衍射、扫描电镜、透射电镜、H₂程序升温还原和O₂程序升温脱附等方法研究了催化剂的结构及物化性质与催化剂活性之间的关系，提出了消除PM反应的可能机理.
结果表明，Al³⁺离子能够部分进入到CeO₂中，形成Al-Ce固溶体.由于Al离子半径小于Ce离子，Al³⁺掺杂后能引起CeO₂晶格发生畸变，产生大量缺陷，形成大量氧空位，促进晶格氧的移动，从而使催化剂具有更大的储放氧能力.在Au/x-CeO₂/3DOM Al₂O₃催化剂中，CeO₂担载量过高时，氧化铈纳米层较厚，活性组分容易烧结，不利于催化剂活性提高；而CeO₂担载量过低，则CeO₂纳米层较稀薄，催化剂的氧化还原性能受限，催化剂活性也不高.因此，CeO₂的担载量应适当.此外，Au和CeO₂之间的强相互作用能够增加Au纳米颗粒表面活性氧物种的数量，从而促进柴油炭烟燃烧反应.活性测试结果表明，担载纳米Au颗粒后，催化剂催化柴油炭烟燃烧的起燃温度均明显降低，在所制备的系列催化剂中Au/20% CeO₂/3DOM Al₂O₃催化剂展示了最高的催化活性，T₁₀，T₅₀和T₉₀分别为267，372和426℃.

关键词: 三维有序大孔材料, 纳米金催化剂, 多层载体, 氧化铈纳米层, 炭烟燃烧

Abstract:

A series of catalysts consisting of three-dimensionally ordered macroporous (3DOM) x-CeO₂/Al₂O₃-supported Au nanoparticles (x=2, 10, 20, and 40 wt%) were successfully synthesized using a reduction-deposition method. These catalysts were characterized using scanning electron microscopy, the Brunauer-Emmett-Teller method, X-ray diffraction, transmission electron micros-copy, ultraviolet-visible spectroscopy, and temperature-programmed reduction by H₂. Au nanopar-ticles of mean particle size 5 nm were well dispersed and supported on the inner walls of uniform macropores. The 3DOM structure improved the contact efficiency between soot and the catalyst. An Al-Ce-O solid solution was formed in the multilayer support, i.e., x-CeO₂/Al₂O₃, by the incorporation of Al³⁺ ions into the CeO₂ lattice, which resulted in the creation of extrinsic oxygen vacancies. Strong interactions between the metal (Au) and the support (Ce) increased the amount of active oxygen species, and this promoted soot oxidation. The catalytic performance in soot combustion was eval-uated using a temperature-programmed oxidation technique. The presence of CeO₂ nanolayers in the 3DOM Au/x-CeO₂/Al₂O₃ catalysts clearly improved the catalytic activities in soot oxidation. Among the prepared catalysts, 3DOM Au/20%CeO₂/Al₂O₃ showed high catalytic activity and stabil-ity in diesel soot oxidation.

Key words: Three-dimensionally ordered macroporous material, Gold nanoparticle, Multilayer support, CeO₂ nanolayer, Soot combustion

靳保芳, 韦岳长, 赵震, 刘坚, 李亚钊, 李人杰, 段爱军, 姜桂元. CeO₂纳米层对多层载体x-CeO₂/3DOM Al₂O₃负载纳米Au催化剂催化柴油炭烟燃烧活性的影响[J]. 催化学报, 2017, 38(9): 1629-1641.

Baofang Jin, Yuechang Wei, Zhen Zhao, Jian Liu, Yazhao Li, Renjie Li, Aijun Duan, Guiyuan Jiang. Three-dimensionally ordered macroporous CeO₂/Al₂O₃-supported Au nanoparticle catalysts:Effects of CeO₂ nanolayers on catalytic activity in soot oxidation[J]. Chinese Journal of Catalysis, 2017, 38(9): 1629-1641.

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CeO₂纳米层对多层载体x-CeO₂/3DOM Al₂O₃负载纳米Au催化剂催化柴油炭烟燃烧活性的影响

Three-dimensionally ordered macroporous CeO₂/Al₂O₃-supported Au nanoparticle catalysts:Effects of CeO₂ nanolayers on catalytic activity in soot oxidation

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