铈酸钡和钇掺杂的铈酸钡复合氧化物的制备及其在钌基氨合成催化剂中的应用  

Preparation and Catalytic Properties of Barium Cerate and Yttrium-Doped Barium Cerate Supported Ruthenium for Ammonia Synthesis

作　　者：杨晓龙[1,2] 夏春谷[1] 熊绪茂[1] 慕新元[1] 胡斌[1] 

机构地区：[1]中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室,甘肃兰州730000 [2]中国科学院研究生院,北京100049

出　　处：《催化学报》2010年第4期377-379,共3页

基　　金：国家自然科学基金(20576025);国家杰出青年科学基金(20625308)

摘　　要：采用柠檬酸法合成了BaCeO3和掺杂Y3+的BaCe0.9Y0.1O3-δ复合氧化物,以Ru3(CO)12为前体,利用浸渍法制备了Ru/BaCeO3和Ru/BaCe0.9Y0.1O3-δ催化剂.通过X射线衍射、扫描电镜和透射电镜技术对样品进行了表征,并在固定床反应器中考察了催化剂的氨合成反应活性.结果表明,载体BaCeO3的稳定性优于BaCe0.9Y0.1O3-δ,但Ru/BaCe0.9Y0.1O3-δ催化剂的氨合成活性明显高于Ru/BaCeO3,在3.0MPa,15000h?1,425oC反应时,Ru/BaCe0.9Y0.1O3-δ催化剂上氨合成反应速率达到432.5ml/(g·h),是Ru/BaCeO3催化剂的1.6倍.这种活性和稳定性的显著差异来自载体中Ce4+与Ru纳米粒子间的电子作用.Barium cerate （BaCeO3） and yttrium-doped barium cerate （BaCe0.9Y0.1O3-δ） were synthesized by the citric acid method and used as supports for Ru/BaCeO3 and Ru/BaCe0.9Y0.1O3-δ catalysts prepared by incipient wetness impregnation using Ru3（CO）12 as precursor. The supports and catalysts were characterized by X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. Their catalytic properties for ammonia synthesis were evaluated in a fixed-bed reactor. The stability of BaCeO3 was superior to that of BaCe0.9Y0.1O3-δ, and the catalytic activity of Ru/BaCe0.9Y0.1O3-δ was higher than that of Ru/BaCeO3. The rate of ammonia synthesis over Ru/BaCe0.9Y0.1O3-δ was 432.5 ml/（g·h） at 3.0 MPa, 425 oC, and 15 000 h-1, which was 1.6 times higher than that of Ru/BaCeO3. The electronic interaction between Ce^4＋ and Ru nanoparticles was the key factor for the difference in catalytic activity and stability.

关 键 词：氨合成 钌 铈酸钡 钇 钙钛矿型氧化物 电子作用 

分 类 号：TQ113.247[化学工程—无机化工]