화학공학소재연구정보센터
Applied Catalysis A: General, Vol.218, No.1-2, 251-256, 2001
The synergistic acceleration of the ammonia synthesis over the K-2[Fe-2(CO)(8)]+K catalysts on carbon "Sibunit" by rhodium
The effect of Rh on the ammonia synthesis over the K-2[Fe-2(CO)(8)]K+ and K-2[Ru-4(CO)(13)]+K catalysts on the graphite-like active carbon "Sibunit" has been investigated. The catalysts were prepared by depositing K-2[Fe-2(CO)(8)] and K-2[Ru-4(CO)(13)]. respectively, onto the "Sibunit" carbon-supported Rh. followed by thermal decomposition of the deposited cluster and treatment of the resulting sample with metallic potassium. The catalysts containing no potassium metal have been studied as well. It has been found that the presence of Rh in the Ru catalysts either little affects the ammonia synthesis rate or even somewhat decreases it. By contrast, the introduction of Rh in the K-2[Fe-2(CO)(8)] + K systems leads to a synergistic acceleration of the process of the ammonia synthesis. The strongest accelerating effects of Rh are observed at lowered temperatures. Thus, at 200 degreesC, the Fe-Rh catalyst (Fe/carbon = 5.6 wt.%, the Fe:Rh molar ratio is 1.6:1) proves to be 3.5 times more active than the corresponding Fe sample. A rise in the reaction temperature to 250, 300 and then to 350 degreesC results in a gradual weakening of the Fe-Rh synergism. A remarkable feature of the Fe-Rh catalyst found is its increased activity in the ammonia formation at 150 degreesC. The analogous Rh catalysts produce no ammonia at all at 150-200 degreesC in the absence of Fe and their efficiency at 250-400 degreesC is either equal to zero or very low.