Halo-oxide ACuO2-δXσ (A = Sr0.63Ca0.27, X = F, Cl) catalysts active and durable for ethane selective oxidation to ethene

H. X. Dai, H. He, C. F. Ng, Chak Tong AU*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

18 Citations (Scopus)

Abstract

The catalytic performance and characterization of ACuO2-δ (A = Sr0.63 Ca0.27) and ACuO2-δXσ (X = F, Cl) catalysts have been investigated for the oxidative dehydrogenation of ethane (ODE) to ethene. The results of X-ray diffraction indicated that the three catalysts are single-phase and tetragonal infinite-layer in structure. The incorporation of fluoride or chloride ions in the ACuO2-δ lattice can significantly enhance C2H6 conversion and C2H4 selectivity. At C2H6/O2/N2 molar ratio = 2/1/3.7 and space velocity = 6000 ml h-1 g-1, we observed 73.5% C2H6 conversion, 67.2% C2H4 selectivity, and 49.4% C2H4 yield at 660°C over ACuO1.901F0.088, and 87.4% C2H6 conversion, 74.4% C2H4 selectivity, and 65.0% C2H4 yield at 680°C over ACuO1.950Cl0.036. With the decrease in C2H6/O2 molar ratio, C2H6 conversion increased, whereas C2H4 selectivity decreased. Within 48 h of on-stream ODE reaction, the two halide-doped materials exhibited sustainable catalytic performance. Based on the results of X-ray photoelectron spectroscopy, O2 temperature-programmed desorption, and C2H6 and C2H6/O2/N2 (2/1/3.7 molar ratio) pulse studies, we conclude that (i) the incorporation of halide ions into the ACuO2-δ lattice could enhance lattice oxygen activity, and (ii) in excessive amount, the O- species accommodated in oxygen vacancies and desorbed below 600°C tend to induce ethane complete oxidation, whereas the lattice oxygen species desorbed above 600°C are active for ethane selective oxidation to ethene. By regulating the oxygen vacancy density and Cu3+ population in the halo-oxide catalyst, one can generate a durable catalyst with good performance for the ODE reaction.

Original languageEnglish
Pages (from-to)217-227
Number of pages11
JournalJournal of Molecular Catalysis A: Chemical
Volume171
Issue number1-2
DOIs
Publication statusPublished - 12 Jun 2001

Scopus Subject Areas

  • Catalysis
  • Process Chemistry and Technology
  • Physical and Theoretical Chemistry

User-Defined Keywords

  • (SrCa)CuOX (X=F,Cl)
  • Ethane oxidative dehydrogenation to ethene
  • Infinite-layer halo-oxide catalyst
  • ODE reaction
  • Superconducting cuprate material
  • XPS characterization

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