催化学报

催化学报 ›› 2008, Vol. 29 ›› Issue (2): 153-158.

• 研究论文 • 上一篇    下一篇

含硫液体烃燃料水蒸气重整制氢II. Pt/Ce0.8Gd0.2O1.9催化剂的原位DRIFTS表征

陈金春,薛青松,路勇,何鸣元   

  1. 华东师范大学化学系, 上海市绿色化学与化工过程绿色化重点实验室, 上海 200062
  • 收稿日期:2008-02-25 出版日期:2008-02-25 发布日期:2012-01-15

H2 Production from Steam Reforming of High Energy Density Motor Fuel with SulfurII. In Situ DRIFTS Studies on Pt/Ce0.8Gd0.2O1.9 Catalyst

CHEN Jinchun, XUE Qingsong, LU Yong*, HE Mingyuan   

  1. Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Department of Chemistry, East China Normal University, Shanghai 200062, China
  • Received:2008-02-25 Online:2008-02-25 Published:2012-01-15

PDF

951

被引次数

16

摘要： 利用原位红外漫反射技术(DRIFTS)对抗硫中毒催化剂Pt/Ce0.8Gd0.2O1.9 (Pt/CGO)上CO吸附、CO/噻吩共吸附以及CO/H2S顺序吸附进行了研究,并与Pt/Al2O3催化剂进行了比较. CO吸附实验表明, 1.6%Pt/CGO-800(800 ℃焙烧)上CO的红外特征吸收峰在2104cm-1, 与1.6%Pt/Al2O3-500上CO的红外特征吸收峰(2070cm-1)相比,向高波数方向移动了34 cm-1. 1.6%Pt/CGO-600上出现两个CO特征吸收峰,主峰位于2108cm-1, 肩峰位于2085cm-1. CO/噻吩共吸附实验表明,噻吩导致1.6%Pt/CGO-800上CO吸附的红外特征吸收峰红移至2090cm-1, 峰强度略有降低; 1.6%Pt/CGO-600上CO的红外特征吸收峰红移至2096cm-1且强度有所降低,同时肩峰消失. 而1.6%Pt/Al2O3-500上CO的红外特征吸收峰明显减弱并红移至2040cm-1. CO/H2S顺序吸附实验表明, H2S导致Pt/CGO催化剂在2104和2108cm-1处的CO特征吸收峰轻微红移,峰强度略有降低,而H2S导致Pt/Al2O3完全丧失CO的吸附能力. 原位DRIFTS表征结果表明, Pt/CGO催化剂上生成的强缺电子特性Pt颗粒具有很强的抗硫中毒能力, 800 ℃焙烧有利于生成单一的抗硫中毒的强缺电子Pt金属位,使得1.6%Pt/CGO-800具有最佳的抗硫中毒性能.

关键词: 原位漫反射红外光谱, 抗硫, 铂催化剂, 制氢, 稀土复合氧化物

Abstract: Sulfur-tolerant Pt/Ce0.8Gd0.2O1.9 (Pt/CGO) and Pt/Al2O3 catalysts were characterized by means of in situ diffuse reflectance infrared fourier transform spectroscopy (DRIFTS) for adsorption of CO and co-adsorption of CO with thiophene and hydrogen sulfide. CO adsorbed on the surface of 1.6%Pt/CGO-800 catalyst (calcined at 800 ℃) showed an IR peak at 2104cm-1, which is 34 cm-1higher than that (2070cm-1) on the surface of 1.6%Pt/Al2O3-500 catalyst. CO adsorbed on the surface of 1.6%Pt/CGO-600 catalyst exhibited two IR peaks, a main peak likewise at 2108cm-1 and a shoulder peak at 2085cm-1. For 1.6%Pt/CGO-800, co-adsorbed thiophene caused a shift of the CO peak from 2104cm-1to 2090cm-1. For 1.6%Pt/CGO-600, the main peak was shifted from 2108cm-1 to 2096cm-1 with a slight reduction of peak intensity, and the shoulder CO peak at2085cm-1disappeared. For 1.6%Pt/Al2O3-500, after thiophene was co-adsorbed, the CO peak at 2070cm-1 shifted about 30 cm-1to a lower wavenumbers and the peak intensity significantly decreased. Subsequently adsorbed H2S only caused a 2-4 cm-1red shift of CO peaks at 2104cm-1 for 1.6%Pt/CGO-800 and 2108cm-1 for 1.6%Pt/CGO-600 but led to a complete loss of the CO adsorption ability of 1.6%Pt/Al2O3-500. These results indicated that strong electron-deficient Pt sites that were resistant to sulfur poison were formed on the Pt/CGO catalysts and calcination at 800 ℃ of Pt/CGO resulted in the formation of unique Pt sites that had the highest sulfur tolerance.

Key words: in situ diffuse reflectance infrared fourier transform spectroscopy, sulfur tolerance, platinum catalyst, hydrogen production, rare earth composite oxide