TY - JOUR
T1 - Synthesis of ethanol from syngas over Rh/MCM-41 Catalyst
T2 - Effect of water on product selectivity
AU - Lopez, Luis
AU - Velasco, Jorge
AU - Montes, Vicente
AU - Marinas, Alberto
AU - Cabrera, Saul
AU - Boutonnet, Magali
AU - Järås, Sven
N1 - Publisher Copyright:
© 2015 by the authors; licensee MDPI, Basel, Switzerland.
PY - 2015
Y1 - 2015
N2 - The thermochemical processing of biomass is an alternative route for the manufacture of fuel-grade ethanol, in which the catalytic conversion of syngas to ethanol is a key step. The search for novel catalyst formulations, active sites and types of support is of current interest. In this work, the catalytic performance of an Rh/MCM-41 catalyst has been evaluated and compared with a typical Rh/SiO2 catalyst. They have been compared at identical reaction conditions (280 °C and 20 bar), at low syngas conversion (2.8%) and at same metal dispersion (H/Rh = 22%). Under these conditions, the catalysts showed different product selectivities. The differences have been attributed to the concentration of water vapor in the pores of Rh/MCM-41. The concentration of water vapor could promote the water-gas-shift-reaction generating some extra carbon dioxide and hydrogen, which in turn can induce side reactions and change the product selectivity. The extra hydrogen generated could facilitate the hydrogenation of a C2-oxygenated intermediate to ethanol, thus resulting in a higher ethanol selectivity over the Rh/MCM-41 catalyst as compared to the typical Rh/SiO2 catalyst; 24% and 8%, respectively. The catalysts have been characterized, before and after reaction, by N2-physisorption, X-ray photoelectron spectroscopy, X-ray diffraction, H2-chemisorption, transmission electron microscopy and temperature programmed reduction.
AB - The thermochemical processing of biomass is an alternative route for the manufacture of fuel-grade ethanol, in which the catalytic conversion of syngas to ethanol is a key step. The search for novel catalyst formulations, active sites and types of support is of current interest. In this work, the catalytic performance of an Rh/MCM-41 catalyst has been evaluated and compared with a typical Rh/SiO2 catalyst. They have been compared at identical reaction conditions (280 °C and 20 bar), at low syngas conversion (2.8%) and at same metal dispersion (H/Rh = 22%). Under these conditions, the catalysts showed different product selectivities. The differences have been attributed to the concentration of water vapor in the pores of Rh/MCM-41. The concentration of water vapor could promote the water-gas-shift-reaction generating some extra carbon dioxide and hydrogen, which in turn can induce side reactions and change the product selectivity. The extra hydrogen generated could facilitate the hydrogenation of a C2-oxygenated intermediate to ethanol, thus resulting in a higher ethanol selectivity over the Rh/MCM-41 catalyst as compared to the typical Rh/SiO2 catalyst; 24% and 8%, respectively. The catalysts have been characterized, before and after reaction, by N2-physisorption, X-ray photoelectron spectroscopy, X-ray diffraction, H2-chemisorption, transmission electron microscopy and temperature programmed reduction.
KW - Ethanol
KW - Rh/MCM-41 catalyst
KW - Syngas
KW - Water vapor
UR - http://www.scopus.com/inward/record.url?scp=84944885472&partnerID=8YFLogxK
U2 - 10.3390/catal5041737
DO - 10.3390/catal5041737
M3 - Artículo
AN - SCOPUS:84944885472
VL - 5
SP - 1737
EP - 1755
JO - Catalysts
JF - Catalysts
SN - 2073-4344
IS - 4
M1 - A08
ER -