TY - JOUR
T1 - Efficient Promoters and Reaction Paths in the CO2Hydrogenation to Light Olefins over Zirconia-Supported Iron Catalysts
AU - Barrios, Alan J.
AU - Peron, Deizi V.
AU - Chakkingal, Anoop
AU - Dugulan, Achim Iulian
AU - Moldovan, Simona
AU - Nakouri, Kalthoum
AU - Thuriot-Roukos, Joëlle
AU - Wojcieszak, Robert
AU - Thybaut, Joris W.
AU - More Authors, null
PY - 2022
Y1 - 2022
N2 - Hydrogenation into light olefins is an attractive strategy for CO2fixation into chemicals. In this article, high throughput experimentation and extended characterization were employed to identify the most efficient promoters and to elucidate structure-performance correlations and reaction paths in the CO2hydrogenation to light olefins over zirconia-supported iron catalysts. K, Cs, Ba, Ce, Nb, Mo, Mn, Cu, Zn, Ga, In, Sn, Sb, Bi, and V were added in the same molar concentrations to zirconia-supported iron catalyst and evaluated as promoters. The CO2hydrogenation proceeds via intermediate formation of CO followed by surface polymerization. Over the iron catalysts containing alkaline promoters, initially higher selectivity to light olefins shows a significant decrease with the CO2conversion, because of further surface polymerization and the formation of longer chain hydrocarbons. A relatively low selectivity to light olefins over the promoted catalysts, without potassium, is not much affected by the CO2conversion. Essential characteristics of iron catalysts to obtain a higher yield of light olefins seem to be a higher iron dispersion, a higher extent of carbidization, and optimized basicity. The strongest promoting effect is reported for the alkaline metals. A further increase in the light olefin selectivity is observed after simultaneous addition of potassium with copper, molybdenum, gallium, or cerium.
AB - Hydrogenation into light olefins is an attractive strategy for CO2fixation into chemicals. In this article, high throughput experimentation and extended characterization were employed to identify the most efficient promoters and to elucidate structure-performance correlations and reaction paths in the CO2hydrogenation to light olefins over zirconia-supported iron catalysts. K, Cs, Ba, Ce, Nb, Mo, Mn, Cu, Zn, Ga, In, Sn, Sb, Bi, and V were added in the same molar concentrations to zirconia-supported iron catalyst and evaluated as promoters. The CO2hydrogenation proceeds via intermediate formation of CO followed by surface polymerization. Over the iron catalysts containing alkaline promoters, initially higher selectivity to light olefins shows a significant decrease with the CO2conversion, because of further surface polymerization and the formation of longer chain hydrocarbons. A relatively low selectivity to light olefins over the promoted catalysts, without potassium, is not much affected by the CO2conversion. Essential characteristics of iron catalysts to obtain a higher yield of light olefins seem to be a higher iron dispersion, a higher extent of carbidization, and optimized basicity. The strongest promoting effect is reported for the alkaline metals. A further increase in the light olefin selectivity is observed after simultaneous addition of potassium with copper, molybdenum, gallium, or cerium.
KW - COmitigation
KW - high throughput
KW - hydrogenation
KW - iron catalysts
KW - light olefins
UR - http://www.scopus.com/inward/record.url?scp=85125952343&partnerID=8YFLogxK
U2 - 10.1021/acscatal.1c05648
DO - 10.1021/acscatal.1c05648
M3 - Article
AN - SCOPUS:85125952343
VL - 12
SP - 3211
EP - 3225
JO - ACS Catalysis
JF - ACS Catalysis
SN - 2155-5435
IS - 5
ER -