催化学报 ›› 2007, Vol. 28 ›› Issue (3): 257-263.

• 研究论文 • 上一篇    下一篇

NOx储存-还原催化剂Pt-Pd/BaO/TiAlO的制备及其抗硫性能

陈英1,何俊2,马玉刚1,陈小平1,王乐夫2,李雪辉2   

  1. 1 茂名学院, 广东茂名 525000; 2 华南理工大学化工与能源学院, 广东广州 510640
  • 收稿日期:2007-03-25 出版日期:2007-03-25 发布日期:2007-03-25

Preparation of Pt-Pd/BaO/TiAlO Catalyst for NOx Storage-Reduction and Its Sulfur Resistance

CHEN Ying1*, HE Jun2, MA Yugang1, CHEN Xiaoping1, WANG Lefu2, LI Xuehui2   

  1. 1 Maoming College, Maoming 525000, Guangdong, China; 2 School of Chemical and Energy Engineering, South China University of Technology, Guangzhou 510640, Guangdong, China
  • Received:2007-03-25 Online:2007-03-25 Published:2007-03-25

摘要: 采用共沉淀-浸渍法制备了新型催化剂Pt-Pd/BaO/TiAlO, 通过对催化剂进行NOx吸附储存实验、有硫(SO2)和无硫情况下的NOx储存-还原循环实验以及程序升温脱附、程序升温还原、 N2吸附-脱附和X射线衍射等表征分析,考察了该催化剂的储存NOx性能以及抗硫性能. 结果表明,在Pt-Pd/BaO/TiAlO中,复合氧化物TiAlO为储存NOx的组分兼载体, Ti和Al原子比为1∶2时,储存NOx能力最大; BaO (4%)作为助剂不但增加了催化剂的热稳定性,还提高了其储存NOx的能力. 与Pt/BaO/γ-Al2O3相比, Pt-Pd/BaO/TiAlO具有良好的抗硫性能. Pt-Pd/BaO/TiAlO上吸附形成的硫化物稳定性较差,易被还原脱除,这是其抗硫性能良好的原因之一.

关键词: 铂, 钯, 氧化钡, 钛铝复合氧化物, 氮氧化物, 储存-还原催化剂, 抗硫性能, 贫燃发动机尾气

Abstract: NOx in exhaust gases from lean burn engines can be clarified over Toyota-type storage-reduction catalysts, but it is difficult for the catalyst to be applied in domestic automobiles due to deterioration caused by SO2 in the emission. A novel Pt-Pd/BaO/TiAlO catalyst for NOx storage-reduction (NSR) was prepared by coprecipitation-impregnation. The catalyst was evaluated by NOx storage in lean burn and by NOx storage-reduction in lean-rich cycles both in the absence and in the presence of SO2, respectively, using a series cyclic sequences of feed which changes from lean conditions (GHSV of 12000 h-1, 800 mg/m3 of NO, 4% of O2, 200 mg/m3 of SO2 for sulfur resistance test, remainder Ar, 350 ℃, and for 30 min) to rich conditions (GHSV of 12000 h-1, 4% of H2, remainder Ar, 350 ℃, and for 20 min). The TiAlO bi-oxide and the catalyst were characterized by temperature-programmed desorption, temperature-programmed reduction, N2 adsorption-desorption, and X-ray diffraction. The results showed that TiAlO bi-oxide in Pt-Pd/BaO/TiAlO catalyst acted as both a support and an adsorbent in the NOx storage-reduction process. The maximum capacity for NOx storage was obtained when the molar ratio of Ti/Al in TiAlO was 1∶2. BaO (4%) not only enhanced the thermal stability of catalyst but also increased NOx storage capacity. Pt-Pd/BaO/TiAlO had better sulfur resistance compared with the Toyota-type NSR catalyst Pt/BaO/γ-Al2O3. One of the reasons might be that sulfur compounds produced in NOx storage on the surface of the catalyst were unstable and easily to be removed by reduction.

Key words: platinum, palladium, barium oxide, titanium-aluminum bi-oxide, nitrogen oxide, storage-reduction catalyst, sulfur resistance, lean burn engine emission