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Pt/TiO_2催化剂上CO氧化反应动力学研究
  • ISSN号:1000-6818
  • 期刊名称:《物理化学学报》
  • 时间:0
  • 分类:O643[理学—物理化学;理学—化学]
  • 作者机构:[1]浙江师范大学物理化学研究所,先进催化材料教育部重点实验室,浙江金华321004
  • 相关基金:国家自然科学基金(21173195)资助项目
中文摘要:

利用沉积沉淀法制备了Pt/TiO2催化剂,将其在不同温度下焙烧,以得到不同颗粒尺寸的Pt.并将这些样品用于CO催化氧化反应以及反应动力学研究.结果表明:焙烧温度对催化剂有明显影响,Pt颗粒尺寸随着焙烧温度的升高而增加;与此同时,CO催化活性随焙烧温度的升高呈先增加后降低的趋势,其中,400℃焙烧的样品表现出最高的催化活性.反应动力学结果表明,催化剂上CO氧化反应表观速率方程为r=5.4×10-7p0.17COp0.36O2,说明在该催化剂上CO氧化遵循Langmuir-Hinshelwood机理.同时,对催化剂进行了CO化学吸附红外光谱和O2化学吸附表征.结果表明,随着焙烧温度的升高,催化剂上CO和O2吸附量均呈现先升高后降低的趋势,这与反应结果和反应动力学方程一致,说明反应受到催化剂表面上CO和O2吸附浓度的影响.而在400℃焙烧的催化剂上,CO和O2吸附量均最高,因此其反应活性也最好.这可能是焙烧过程影响了Pt和TiO2之间的相互作用引起的.

英文摘要:

A series of Pt/TiO2 catalysts were prepared using a deposition-precipitation method and calcined at different temperatures to obtain various Pt particle sizes. The catalysts were tested for catalytic CO oxidation and the kinetics of the reaction was studied. The results showed that the Pt particle size increased with calcination temperature, and that their reactivity for CO oxidation first increased and then decreased with increasing calcination temperature, with the catalyst calcined at 400 ℃ possessing the highest by r=5.4×10^-7 pco^0.17 po2^0.36 , reactivity. The kinetic investigation revealed that the reaction rate could be described suggesting that the reaction followed a Langmuir-Hinshelwood mechanism. Meanwhile, 02 chemisorption and infrared (IR) spectroscopy of CO chemisorption on the catalysts were conducted to reveal the relationship between the catalyst structure and its catalytic behavior. It was found that the amount of 02 chemisorption and the intensity of CO chemisorption by IR on the catalysts first increased and then decreased with increasing calcination temperature, which was consistent with the catalytic results and the kinetic equation. This could explain the catalytic behaviors of the catalysts. For example, the highest amounts of chemisorbed O2 and CO were obtained over the PtFFiO2 calcined at 400 ℃, which resulted in the highest reactivity. Such an enhancement in reactivity was probably due to the strong interaction between Pt and TiO2 induced by the calcination process.

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期刊信息
  • 《物理化学学报》
  • 中国科技核心期刊
  • 主管单位:中国科学技术协会
  • 主办单位:北京大学化学与分子工程学院承办
  • 主编:刘忠范
  • 地址:北京大学化学楼
  • 邮编:100871
  • 邮箱:whxb@pku.edu.cn
  • 电话:010-62751724
  • 国际标准刊号:ISSN:1000-6818
  • 国内统一刊号:ISSN:11-1892/O6
  • 邮发代号:82-163
  • 获奖情况:
  • 中文核心期刊
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国科学引文索引(扩展库),英国科学文摘数据库,日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:24781