含硫液体烃燃料水蒸气重整制氢 Ⅱ. Pt/Ce_(0.8)Gd_(0.2)O_(1.9)催化剂的原位DRIFTS表征  

H_2 Production from Steam Reforming of High Energy Density Motor Fuel with Sulfur Ⅱ. In Situ DRIFTS Studies on Pt/Ce_(0.8)Gd_(0.2)O_(1.9) Catalyst

作　　者：陈金春[1] 薛青松[1] 路勇[1] 何鸣元[1] 

机构地区：[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

出　　处：《催化学报》2008年第2期153-158,共6页

基　　金：国家自然科学基金(20590366,20573036);上海市重点学科建设项目(B409);教育部“新世纪优秀人才支持计划”项目(NCET-06-0423);上海市教育发展基金会“曙光计划”项目(06SG28)

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34cm-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.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 17） showed an IR peak at 2104 cm^-1, which is 34 cm^-1 higher than that （2 070 cm^-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 2 108 cm^-1 and a shoulder peak at 2 085 cm ^-1. For 1.6%Pt/CGO-800, co-adsorbed thiophene caused a shift of the CO peak from 2 104 cm^-1 to 2 090 cm^-1. For 1.6%Pt/CGO-600, the main peak was shifted from 2 108 cm^- 1 to 2 096 cm^ -1 with a slight reduction of peak intensity, and the shoulder CO peak at 2 085 cm 1 disappeared. For 1.6 % Pt/Al2O3-500, after thiophene was co-adsorbed, the CO peak at 2 070 cm^-1 shifted about 30 cm^-1 to lower wavenumbers, and the peak intensity significantly decreased. Subsequently, adsorbed H2S only caused a 2 4 cm^- 1 red shift of CO peaks at 2 104 cm^- 1 for 1.6 % Pt/CGO-800 and 2 108 cm^-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.

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 

分 类 号：TQ116.2[化学工程—无机化工] O643.32[理学—物理化学]