TY - JOUR
T1 - Insights into the structure–activity relationship in aqueous-phase hydrogenation of levulinic acid to 1,4-pentanediol over bimetallic Ru-Re/C catalysts
AU - Lee, Dongju
AU - Kim, Han Ung
AU - Kim, Jung Rae
AU - Park, Young Kwon
AU - Ha, Jeong Myeong
AU - Jae, Jungho
N1 - Publisher Copyright:
© 2023 The Korean Society of Industrial and Engineering Chemistry
PY - 2024/3/25
Y1 - 2024/3/25
N2 - Hydrogenation of biomass-derived levulinic acid (LA) to 1,4-pentanediol (PDO) is a sustainable route to replace petroleum-derived polyols. Although the combination of ruthenium (Ru), a hydrogenating metal, and rhenium (Re), an oxophilic promoter, results in high activity for PDO production, the synergistic effect between Ru and Re and the effect of carbon support are not well understood. In this study, the factors determining the catalytic activity and selectivity of carbon-supported RuRe for PDO production were investigated. Bimetallic RuRe nanoparticles with various atomic ratios and monometallic Ru and Re were supported on various carbon materials with different surface properties such as activated carbon (AC), carbon black (CB), mesoporous carbon (CMK-3), carbon nanofiber (CNF) and their reaction kinetics were compared. The structural and physicochemical properties of the catalysts were characterized using X-ray diffraction, temperature-programmed reduction, N2-physisorption, transmission electron microscopy, and X-ray photoelectron spectroscopy. The catalytic activity and PDO selectivity were correlated with the metal particle size, pore structure, and surface oxygen functionalities, in which the smaller RuRe nanoparticles with a Re-enriched surface supported on carbon with a larger pore size exhibited a higher PDO production rate. Among the catalysts, RuRe supported on CB exhibited the highest PDO selectivity (∼75 %) at 130 °C and 50 bar-H2. The impact of the Re promoter in the RuRe/C catalyst on the LA hydrogenation mechanism was also investigated for the first time using in situ FT-IR spectroscopy.
AB - Hydrogenation of biomass-derived levulinic acid (LA) to 1,4-pentanediol (PDO) is a sustainable route to replace petroleum-derived polyols. Although the combination of ruthenium (Ru), a hydrogenating metal, and rhenium (Re), an oxophilic promoter, results in high activity for PDO production, the synergistic effect between Ru and Re and the effect of carbon support are not well understood. In this study, the factors determining the catalytic activity and selectivity of carbon-supported RuRe for PDO production were investigated. Bimetallic RuRe nanoparticles with various atomic ratios and monometallic Ru and Re were supported on various carbon materials with different surface properties such as activated carbon (AC), carbon black (CB), mesoporous carbon (CMK-3), carbon nanofiber (CNF) and their reaction kinetics were compared. The structural and physicochemical properties of the catalysts were characterized using X-ray diffraction, temperature-programmed reduction, N2-physisorption, transmission electron microscopy, and X-ray photoelectron spectroscopy. The catalytic activity and PDO selectivity were correlated with the metal particle size, pore structure, and surface oxygen functionalities, in which the smaller RuRe nanoparticles with a Re-enriched surface supported on carbon with a larger pore size exhibited a higher PDO production rate. Among the catalysts, RuRe supported on CB exhibited the highest PDO selectivity (∼75 %) at 130 °C and 50 bar-H2. The impact of the Re promoter in the RuRe/C catalyst on the LA hydrogenation mechanism was also investigated for the first time using in situ FT-IR spectroscopy.
KW - 1,4-pentanediol
KW - Bimetallic
KW - Biomass
KW - Levulinic acid
KW - RuRe
UR - http://www.scopus.com/inward/record.url?scp=85176449505&partnerID=8YFLogxK
U2 - 10.1016/j.jiec.2023.10.053
DO - 10.1016/j.jiec.2023.10.053
M3 - Article
AN - SCOPUS:85176449505
SN - 1226-086X
VL - 131
SP - 490
EP - 502
JO - Journal of Industrial and Engineering Chemistry
JF - Journal of Industrial and Engineering Chemistry
ER -