催化学报

催化学报 ›› 2012, Vol. 33 ›› Issue (6): 907-913.DOI: 10.1016/S1872-2067(11)60402-6

• 研究论文 • 上一篇    下一篇

Zr 掺杂对 La(Ba)ZrxCo1-xO3-δ 钙钛矿催化 N2O 分解性能的影响

刘爽 1,2, 丛昱 1, Charles KAPPENSTEIN1,3, 张涛 1,*   

  1. 1 中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连 116023; 2 中国科学院研究生院, 北京 100049; 3 普瓦提大学环境与材料化学研究所, 法国普瓦提 86022
  • 收稿日期:2012-03-15 修回日期:2012-04-12 出版日期:2012-05-30 发布日期:2012-05-30

Effect of Zirconium in La(Ba)ZrxCo1-xO3-δ Perovskite Catalysts for N2O Decomposition

LIU Shuang1,2, CONG Yu1, Charles KAPPENSTEIN1,3, ZHANG Tao1,*   

  1. 1 State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China; 2 Graduate University of Chinese Academy of Sciences, Beijing 100049, China; 3 Institute of Chemistry of Mediums and Materials of Poitiers, University of Poitiers, Poitiers 86022, France
  • Received:2012-03-15 Revised:2012-04-12 Online:2012-05-30 Published:2012-05-30

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摘要： 采用溶胶凝胶法制备了 Zr 掺杂的钴基钙钛矿 La(Ba)ZrxCo1-xO3-δ, 并将其用于航天推进剂领域的高浓度 N2O 催化分解反应. 发现 Zr 的引入明显提高了钙钛矿 La(Ba)ZrxCo1-xO3-δ的催化活性, 尤其是当 Zr 掺杂量分别为 0.05 和 0.2 时, LaZrxCo1-xO3-δ和 BaZrxCo1-xO3-δ催化剂性能较为优异. 应用 N2 物理吸附、X 射线衍射、H2 程序升温还原、O2 程序升温脱附和氧脉冲吸附技术表征了 Zr 掺杂对 La(Ba)ZrxCo1-xO3-δ 催化剂的物化性质的影响. 结果表明, Zr 掺杂增大了钴基钙钛矿的比表面积, 改善了晶格结构, 从而提高了钴物种的还原及氧吸附脱附能力, 因而催化剂上 N2O 分解活性增加.

关键词: 钴酸镧, 钴酸钡, 锆, 氧化亚氮, 分解

Abstract: Zr-incorporated La(Ba)ZrxCo1-xO3-δ perovskites were prepared by a sol-gel method and used for the catalytic decomposition of the high concentrations of N2O present in propulsion applications. The introduction of Zr significantly enhanced N2O conversion, esp. with x = 0.05 and 0.2 for LaZrxCo1-xO3-δ and BaZrxCo1-xO3-δ, respectively. N2 adsorption, X-ray diffraction, temperature-programmed reduction of H2, temperature-programmed desorption of O2, and oxygen pulse chemisorption techniques were used to characterize the structure and redox and oxygen adsorption property of the perovskites. The increasing of the surface area, modifying of the crystal structure, more facile reducibility of cobalt species, and higher oxygen desorption-adsorption activity due to the introduction of Zr were the reasons for the activity enhancement for N2O decomposition.

Key words: lanthanum cobaltate, barium cobaltate, zirconium, nitrous oxide, decomposition