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作 者:刘爽[1,2] 丛昱[1] Charles KAPPENSTEIN 张涛[1]
机构地区:[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
出 处:《催化学报》2012年第6期907-913,共7页
基 金:supported by the National Natural Science Foundation of China (20973165);the External Cooperation Program of Chinese Academy of Sciences (GJHZ200827)~~
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.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.
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