화학공학소재연구정보센터
Applied Catalysis A: General, Vol.209, No.1-2, 317-325, 2001
Rhenium containing binary catalysts for ammonia synthesis
The rhenium nitride was prepared and applied for ammonia synthesis. Under the synthesis conditions (623 K, 0.1 MPa), the nitride was partly decomposed (Re3N + Re) but the activity was stable and higher (179 mu mol h(-1) g(-1) at 623 K under 0.1 MPa) than the other transition metal nitrides (VN, NbN, Mo2N, and W2N), although the BET surface area was immeasurably low. The active phase was considered to be Re3N. The effect of transition metal addition to the rhenium catalyst for ammonia synthesis was investigated. Cobalt and iron were effective, but nickel, chromium, and copper were not effective. The best combination was Go-Re (1:4) (492 mu mol h(-1) g(-1) at 623 K under 0.1 MPa, expressed as Co-Re-4 catalyst). NH3 treatment of Co-Re-4 at 973 K gave a new XRD pattern (probably some kind of rhenium nitride phase), which was suggested to be responsible to the high activity of Co-Re4 catalyst. The ammonia synthesis rate over Co-Re4 catalyst was increased under high pressure (2372 mu mol h(-1) g(-1) at 623 K under 3.1 MPa), however, the rate overshot above 1.1 MPa. The kinetic analysis indicated that Re surface was strongly covered either by hydrogen or by nitrogen (ammonia). By the addition of cobalt, the degree of nitrogen (ammonia) poisoning was weakened, but at the same time, the degree of hydrogen poisoning was strengthened.