TY - JOUR
T1 - Halo-oxide ACuO2-δXσ (A = Sr0.63Ca0.27, X = F, Cl) catalysts active and durable for ethane selective oxidation to ethene
AU - Dai, H. X.
AU - He, H.
AU - Ng, C. F.
AU - Au, C. T.
N1 - Funding Information:
The work described in this paper was fully supported by a grant from the Research Grants Council of the Hong Kong Special Administration Region, China (project no. HKBU 2015/99P).
PY - 2001/6/12
Y1 - 2001/6/12
N2 - 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.
AB - 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.
KW - (SrCa)CuOX (X=F,Cl)
KW - Ethane oxidative dehydrogenation to ethene
KW - Infinite-layer halo-oxide catalyst
KW - ODE reaction
KW - Superconducting cuprate material
KW - XPS characterization
UR - http://www.scopus.com/inward/record.url?scp=0035849502&partnerID=8YFLogxK
U2 - 10.1016/S1381-1169(01)00105-4
DO - 10.1016/S1381-1169(01)00105-4
M3 - Journal article
AN - SCOPUS:0035849502
SN - 1381-1169
VL - 171
SP - 217
EP - 227
JO - Journal of Molecular Catalysis A: Chemical
JF - Journal of Molecular Catalysis A: Chemical
IS - 1-2
ER -