In-situ FT-IR study of CO hydrogenation to C2 oxygenates over Rh-based catalysts

被引:0
作者
Yin, HM [1 ]
Ding, YJ [1 ]
Luo, HY [1 ]
He, DP [1 ]
Xiong, JM [1 ]
Chen, WM [1 ]
Pan, ZD [1 ]
Lin, LW [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Liaoning, Peoples R China
关键词
rhodium-based catalyst; carbon monoxide; hydrogenation; C-2; oxygenate; in-situ infrared spectroscopy;
D O I
暂无
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
In-situ FT-IR technique was employed to investigate CO adsorption and the changes of adsorbed species on the surface of Rh-based catalysts during CO hydrogenation. The result showed that only the linear CO was observed on Rh/SiO2, while linear CO and twin CO appeared on Rh-Mn-Li-Fe/SiO2, indicating that Rh dispersion on Rh-Mn-Li-Fe/SiO2 was higher than that on Rh/SiO2. In the IR spectra of CO hydrogenation under the conditions of 593 K and 3.0 MPa, the bands at 1 716, 1566, 1442, and 1 343 cm which were attributed to C-2 oxygenate precursors, were observed for Rh-Mn-Li-Fe/SiO2, while no band was detected for Rh/SiO2. CO was adsorbed mainly as linear CO on both the catalysts during CO hydrogenation. Correlating the FTIR results with the CO hydrogenation performance suggested that the linear CO might be mainly responsible for the formation of C-2 oxygenates. The high activity of Rh-Mn-Li-Fe/SiO2 was due to the fact that the existence of promoters weakened the C-O bond of adsorbed CO on the catalyst, promoted CO activation and favored the formation of C-2-oxygenate intermediates under the reaction conditions.
引用
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页码:547 / 550
页数:4
相关论文
共 18 条
[1]   NOVEL HIGH-PRESSURE FT-IR SPECTROSCOPIC SYSTEM COMBINED WITH SPECIALLY DESIGNED INSITU IR CELL FOR STUDYING HETEROGENEOUS CATALYTIC REACTIONS [J].
ARAKAWA, H ;
FUKUSHIMA, T ;
ICHIKAWA, M .
APPLIED SPECTROSCOPY, 1986, 40 (06) :884-886
[2]   SELECTIVE SYNTHESIS OF ETHANOL OVER RH-TI-FE-IR/SIO2 CATALYST AT HIGH-PRESSURE SYNGAS CONVERSION [J].
ARAKAWA, H ;
FUKUSHIMA, T ;
ICHIKAWA, M ;
NATSUSHITA, S ;
TAKEUCHI, K ;
MATSUZAKI, T ;
SUGI, Y .
CHEMISTRY LETTERS, 1985, (07) :881-884
[3]   SYNTHESIS GAS CONVERSION OVER SUPPORTED RHODIUM AND RHODIUM-IRON CATALYSTS [J].
BHASIN, MM ;
BARTLEY, WJ ;
ELLGEN, PC ;
WILSON, TP .
JOURNAL OF CATALYSIS, 1978, 54 (02) :120-128
[4]   CO-INDUCED STRUCTURAL-CHANGES OF RH ON TIO2 SUPPORT [J].
BUCHANAN, DA ;
HERNANDEZ, ME ;
SOLYMOSI, F ;
WHITE, JM .
JOURNAL OF CATALYSIS, 1990, 125 (02) :456-466
[5]   IN-SITU FTIR STUDY OF CO-H-2 REACTIONS OVER RH/TIO2 CATALYSTS AT HIGH-PRESSURE AND TEMPERATURE [J].
CHUDEK, JA ;
MCQUIRE, MW ;
MCQUIRE, GW ;
ROCHESTER, CH .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1994, 90 (24) :3699-3709
[6]   INSITU HIGH-PRESSURE FT IR STUDIES ON THE SURFACE SPECIES FORMED IN CO HYDROGENATION ON SIO2-SUPPORTED RH-FE CATALYSTS [J].
FUKUSHIMA, T ;
ARAKAWA, H ;
ICHIKAWA, M .
JOURNAL OF PHYSICAL CHEMISTRY, 1985, 89 (21) :4440-4443
[7]   HIGH-PRESSURE IR SPECTROSCOPIC EVIDENCE OF ACETYL AND ACETATE SPECIES DIRECTLY FORMED IN CO-H2 CONVERSION ON SIO2-SUPPORTED RH AND RH-MN CATALYSTS [J].
FUKUSHIMA, T ;
ARAKAWA, H ;
ICHIKAWA, M .
JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1985, (11) :729-731
[8]  
JOHNSTON P, 1990, FARADAY DISCUSS, V89, P91
[9]   THE ROLE OF THE SUPPORT IN CO HYDROGENATION SELECTIVITY OF SUPPORTED RHODIUM [J].
KATZER, JR ;
SLEIGHT, AW ;
GAJARDO, P ;
MICHEL, JB ;
GLEASON, EF ;
MCMILLAN, S .
FARADAY DISCUSSIONS, 1981, 72 :121-133
[10]   VANADIUM-OXIDE AS A SUPPORT AND PROMOTER OF RHODIUM IN SYNTHESIS GAS REACTIONS [J].
KOWALSKI, J ;
VANDERLEE, G ;
PONEC, V .
APPLIED CATALYSIS, 1985, 19 (02) :423-426