TY - JOUR
T1 - Performance and characterization of rhenium-modified Rh-Ir alloy catalyst for one-pot conversion of furfural into 1,5-pentanediol
AU - Liu, Sibao
AU - Amada, Yasushi
AU - Tamura, Masazumi
AU - Nakagawa, Yoshinao
AU - Tomishige, Keiichi
PY - 2014/8
Y1 - 2014/8
N2 - One-pot selective conversion of highly concentrated furfural to 1,5-pentanediol (1,5-PeD) was carried out over Rh-added Ir-ReO x/SiO2 catalysts through two-step reaction temperatures. Over the optimized catalyst, Rh(0.66 wt%)-Ir-ReOx/SiO2, the maximum yield of 1,5-PeD was 71.1% from highly concentrated furfural (50 wt%) and 78.2% from diluted furfural (10 wt%). These values were higher than those obtained with Ir-ReOx/SiO2 or Pd-Ir-ReO x/SiO2 catalysts. Rh-Ir-ReOx/SiO2 showed much higher activity in the hydrogenation of furfural to tetrahydrofurfuryl alcohol intermediate in the low temperature step than Ir-ReOx/SiO2, although the hydrogenation activity was lower than that of Pd-Ir-ReOx/SiO2. A long reaction time in the low temperature step is necessary to obtain a good 1,5-PeD yield over Rh-Ir-ReOx/SiO2 in two-step reaction of furfural. The hydrogenolysis activity of Rh-Ir-ReOx/SiO2 for tetrahydrofurfuryl alcohol to 1,5-PeD in the high temperature step was higher than that of Pd-Ir-ReOx/SiO2 and was comparable to that of Ir-ReOx/SiO2. The characterization results of TPR, XRD, XANES, EXAFS, STEM-EDX and FT-IR of adsorbed CO indicated that Rh-Ir-ReO x/SiO2 catalysts showed the structure of Ir-Rh alloy particles partially covered with ReOx species. The hydrogenation activity of Rh-Ir-ReOx/SiO2 for the furan ring was higher than those of the mixture of Rh-Ir/SiO2 and Ir-ReO x/SiO2 or the mixture of Rh-ReOx/SiO 2 and Ir-ReOx/SiO2. Both Ir-Rh alloy formation and ReOx modification of alloy particles are essential for the high hydrogenation activity.
AB - One-pot selective conversion of highly concentrated furfural to 1,5-pentanediol (1,5-PeD) was carried out over Rh-added Ir-ReO x/SiO2 catalysts through two-step reaction temperatures. Over the optimized catalyst, Rh(0.66 wt%)-Ir-ReOx/SiO2, the maximum yield of 1,5-PeD was 71.1% from highly concentrated furfural (50 wt%) and 78.2% from diluted furfural (10 wt%). These values were higher than those obtained with Ir-ReOx/SiO2 or Pd-Ir-ReO x/SiO2 catalysts. Rh-Ir-ReOx/SiO2 showed much higher activity in the hydrogenation of furfural to tetrahydrofurfuryl alcohol intermediate in the low temperature step than Ir-ReOx/SiO2, although the hydrogenation activity was lower than that of Pd-Ir-ReOx/SiO2. A long reaction time in the low temperature step is necessary to obtain a good 1,5-PeD yield over Rh-Ir-ReOx/SiO2 in two-step reaction of furfural. The hydrogenolysis activity of Rh-Ir-ReOx/SiO2 for tetrahydrofurfuryl alcohol to 1,5-PeD in the high temperature step was higher than that of Pd-Ir-ReOx/SiO2 and was comparable to that of Ir-ReOx/SiO2. The characterization results of TPR, XRD, XANES, EXAFS, STEM-EDX and FT-IR of adsorbed CO indicated that Rh-Ir-ReO x/SiO2 catalysts showed the structure of Ir-Rh alloy particles partially covered with ReOx species. The hydrogenation activity of Rh-Ir-ReOx/SiO2 for the furan ring was higher than those of the mixture of Rh-Ir/SiO2 and Ir-ReO x/SiO2 or the mixture of Rh-ReOx/SiO 2 and Ir-ReOx/SiO2. Both Ir-Rh alloy formation and ReOx modification of alloy particles are essential for the high hydrogenation activity.
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U2 - 10.1039/c4cy00161c
DO - 10.1039/c4cy00161c
M3 - Article
AN - SCOPUS:84904112127
SN - 2044-4753
VL - 4
SP - 2535
EP - 2549
JO - Catalysis Science and Technology
JF - Catalysis Science and Technology
IS - 8
ER -