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.
出处
《催化学报》
SCIE
EI
CAS
CSCD
北大核心
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)
关键词
氨合成
钌
铈酸钡
钇
钙钛矿型氧化物
电子作用
ammonia synthesis
ruthenium
barium cerate
yttrium
perovskite-type oxide
electronic interaction
