The effects of PVP-modified SiO2 on the catalytic performance of CO hydrogenation over Rh-Mn-Li/SiO2 catalysts

被引:11
作者
Ding, Dan [1 ]
Yu, Jun [1 ]
Guo, Qiangsheng [1 ]
Guo, Xiaoming [1 ]
Xiao, Xiuzhen [1 ]
Mao, Dongsen [1 ]
Lu, Guanzhong [1 ]
机构
[1] Shanghai Inst Technol, Sch Chem & Environm Engn, Res Inst Appl Catalysis, Shanghai 201418, Peoples R China
关键词
SUPPORTED RH CATALYSTS; C-2-OXYGENATES SYNTHESIS; RHODIUM CATALYSTS; ETHANOL SYNTHESIS; SYNGAS; CONVERSION; SILICA; PROMOTER; MN; FE;
D O I
10.1039/c7ra07011j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Rh-Mn-Li catalysts supported on SiO2 prepared by PVP-modified Stober method were used for the synthesis of C-2(+) oxygenates from CO hydrogenation. The catalysts were characterized by TG, XRD, N-2-adsorption-desorption, TEM, H-2-TPR, in situ FT-IR, TPSR, and XPS. Activity testing results showed that the Rh-Mn-Li catalyst supported on the SiO2 modified by 1 g PVP exhibited the highest CO conversion and selectivity of C-2(+) oxygenates compared with other catalysts. Characterization results indicated that the addition of an appropriate amount of PVP is beneficial to the formation of weakly H-bonded hydroxyl groups on the surface of SiO2, which promotes Rh dispersion and weakens the Rh-Mn interaction. Furthermore, the higher Rh dispersion and the weaker Rh-Mn interaction promote CO absorption, enhance the CO dissociation ability and restrain the hydrogenation activity, which are favorable for the CO insertion into the metal-CHX band, finally resulting in excellent catalytic performance for C2+D oxygenates synthesis.
引用
收藏
页码:48420 / 48428
页数:9
相关论文
共 35 条
[1]   SPECTROSCOPIC EVIDENCE FOR THE INVOLVEMENT OF OH GROUPS IN THE FORMATION OF RHI(CO)2 ON METAL-OXIDE SUPPORTS [J].
BASU, P ;
PANAYOTOV, D ;
YATES, JT .
JOURNAL OF PHYSICAL CHEMISTRY, 1987, 91 (12) :3133-3136
[2]   RHODIUM CARBON-MONOXIDE SURFACE-CHEMISTRY - THE INVOLVEMENT OF SURFACE HYDROXYL-GROUPS ON AL2O3 AND SIO2 SUPPORTS [J].
BASU, P ;
PANAYOTOV, D ;
YATES, JT .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1988, 110 (07) :2074-2081
[3]   Direct conversion of syngas to ethanol over Rh/Mn-supported on modified SBA-15 molecular sieves: Effect of supports [J].
Chen, Guochang ;
Guo, Cun-Yue ;
Zhang, Xiaohui ;
Huang, Zhijun ;
Yuan, Guoqing .
FUEL PROCESSING TECHNOLOGY, 2011, 92 (03) :456-461
[4]   An effective method of controlling metal particle size on impregnated Rh-Mn-Li/SiO2 catalyst [J].
Chen, WM ;
Ding, YJ ;
Jiang, DH ;
Pan, ZD ;
Luo, HY .
CATALYSIS LETTERS, 2005, 104 (3-4) :177-180
[5]   Mechanism of Ethanol Synthesis from Syngas on Rh(111) [J].
Choi, YongMan ;
Liu, Ping .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (36) :13054-13061
[6]   Catalytic conversion of syngas into C2 oxygenates over Rh-based catalysts-Effect of carbon supports [J].
Fan, Zhongli ;
Chen, Wei ;
Pan, Xiulian ;
Bao, Xinhe .
CATALYSIS TODAY, 2009, 147 (02) :86-93
[7]   Synthesis of Ethanol via Syngas on Cu/SiO2 Catalysts with Balanced Cu0-Cu+ Sites [J].
Gong, Jinlong ;
Yue, Hairong ;
Zhao, Yujun ;
Zhao, Shuo ;
Zhao, Li ;
Lv, Jing ;
Wang, Shengping ;
Ma, Xinbin .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (34) :13922-13925
[8]   Fe-promotion of supported Rh catalysts for direct conversion of syngas to ethanol [J].
Haider, Mohammad A. ;
Gogate, Makarand R. ;
Davis, Robert J. .
JOURNAL OF CATALYSIS, 2009, 261 (01) :9-16
[9]   C2-oxygenates synthesis through CO hydrogenation on SiO2-ZrO2 supported Rh-based catalyst: The effect of support [J].
Han, Lupeng ;
Mao, Dongsen ;
Yu, Jun ;
Guo, Qiangsheng ;
Lu, Guanzhong .
APPLIED CATALYSIS A-GENERAL, 2013, 454 :81-87
[10]   Effects of ethanol impregnation on the properties of silica-supported cobalt catalysts [J].
Ho, SW ;
Su, YS .
JOURNAL OF CATALYSIS, 1997, 168 (01) :51-59