TY - JOUR
T1 - Interaction of hydrogen with Cu-Zn mixed oxide model methanol synthesis catalyst
AU - Khassin, Alexander A.
AU - Jobic, Hervé
AU - Filonenko, Georgiy A.
AU - Dokuchits, Evgeniy V.
AU - Khasin, Alexander V.
AU - Minyukova, Tatyana P.
AU - Shtertser, Natalia V.
AU - Plyasova, Lyudmila M.
AU - Yurieva, Tamara M.
PY - 2013
Y1 - 2013
N2 - Interaction of hydrogen with model Cu-Zn methanol synthesis catalyst prepared by decomposition of mixed hydroxicarbonate is studied by inelastic neutron scattering, in situ FTIR/MS, and thermal analysis. Reduced (Cu 0.08,Zn0.92)O mixed oxide accumulates 6H/Cu, mainly as hydride, hydroxyl and formate species. The reduction of copper in the (Cu,Zn)O mixed oxide occurs via a reversible redox interaction with H2 and absorption of protons as OH--groups with ν = 3250 cm-1 and δ ≈ 1430-1480 cm-1. Kinetic and thermodynamic parameters of this process are evaluated. The weight loss during the reduction is due to the decomposition of the residual carbonate groups to CO2 via formate intermediates, which occurs in the presence of hydrogen. Exposure of (Cu,Zn)O to air prior to the reduction strongly affects the kinetic parameters of the reduction process.
AB - Interaction of hydrogen with model Cu-Zn methanol synthesis catalyst prepared by decomposition of mixed hydroxicarbonate is studied by inelastic neutron scattering, in situ FTIR/MS, and thermal analysis. Reduced (Cu 0.08,Zn0.92)O mixed oxide accumulates 6H/Cu, mainly as hydride, hydroxyl and formate species. The reduction of copper in the (Cu,Zn)O mixed oxide occurs via a reversible redox interaction with H2 and absorption of protons as OH--groups with ν = 3250 cm-1 and δ ≈ 1430-1480 cm-1. Kinetic and thermodynamic parameters of this process are evaluated. The weight loss during the reduction is due to the decomposition of the residual carbonate groups to CO2 via formate intermediates, which occurs in the presence of hydrogen. Exposure of (Cu,Zn)O to air prior to the reduction strongly affects the kinetic parameters of the reduction process.
KW - Copper reduction
KW - Copper-zinc oxide catalyst
KW - Hydrogen absorption
KW - In situ FTIR
KW - Inelastic neutron scattering
UR - http://www.scopus.com/inward/record.url?scp=84876932094&partnerID=8YFLogxK
U2 - 10.1016/j.molcata.2013.03.014
DO - 10.1016/j.molcata.2013.03.014
M3 - Article
AN - SCOPUS:84876932094
SN - 1381-1169
VL - 373
SP - 151
EP - 160
JO - Journal of Molecular Catalysis A: Chemical
JF - Journal of Molecular Catalysis A: Chemical
ER -