Effect of PdIn bimetallic particle formation on CO2 reduction over the Pd-In/SiO2 catalyst

被引:105
作者
Ye, Jingyun [1 ,2 ]
Ge, Qingfeng [1 ,2 ,3 ]
Liu, Chang-jun [1 ,2 ]
机构
[1] Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn, Tianjin 300072, Peoples R China
[2] Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300072, Peoples R China
[3] So Illinois Univ, Dept Chem & Biochem, Carbondale, IL 62901 USA
基金
中国国家自然科学基金;
关键词
CO2; reduction; Reverse water gas shift; Bimetallic nanoparticles; Palladium; In2O3; DFT; METHANOL SYNTHESIS; REFORMING ACTIVITY; CARBON-DIOXIDE; HYDROGENATION; METHANATION; ADSORPTION; CHEMISORPTION; SELECTIVITY; SURFACE; DFT;
D O I
10.1016/j.ces.2015.04.034
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
A Pd-In/SiO2 catalyst was prepared by the wet impregnation method and used for CO2 reduction at atmospheric pressure. The catalyst was shown to have 100% selectivity toward CO with no detectable CH4 formation. In order to understand the high CO selectivity of Pd-In/SiO2, a detailed catalyst characterization in combination with the DFT study was conducted and compared with that over the Pd/SiO2 catalyst. The XRD and TEM analyses indicate the formation of the PdIn bimetallic nanoparticles on Pd-In/SiO2 after H-2 reduction. The unique catalytic property of Pd-In/SiO2 was attributed to the formation of the bimetallic particles. Characterizations including H-2 chemisorption and DRIFT and DFT modeling show that the formation of PdIn bimetallic nanoparticles reduces the activity toward H-2 dissociative adsorption, weakens CO binding on the surface and increases the barrier of CO hydrogenation, suppressing the further hydrogenation beyond CO. (C) 2015 Elsevier Ltd. All rights reserved.
引用
收藏
页码:193 / 201
页数:9
相关论文
共 45 条
[1]   Interaction between nickel and molybdenum in Ni-Mo/Al2O3 catalysts:: I -: CO2 methanation and SEM-TEM studies [J].
Aksoylu, AE ;
Misirli, Z ;
Onsan, ZI .
APPLIED CATALYSIS A-GENERAL, 1998, 168 (02) :385-397
[2]   Electrocatalytic CO2 Conversion to Oxalate by a Copper Complex [J].
Angamuthu, Raja ;
Byers, Philip ;
Lutz, Martin ;
Spek, Anthony L. ;
Bouwman, Elisabeth .
SCIENCE, 2010, 327 (5963) :313-315
[3]   Direct IR observation of vibrational properties of carbonyl species formed on Pd nano-particles supported on amorphous carbon:: comparison with Pd/SiO2-Al2O3 [J].
Bertarione, S. ;
Prestipino, C. ;
Groppo, E. ;
Scarano, D. ;
Spoto, G. ;
Zecchina, A. ;
Pellegrini, R. ;
Leofanti, G. ;
Lamberti, C. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2006, 8 (31) :3676-3681
[4]   Surface reactivity of Pd nanoparticles supported on polycrystalline substrates as compared to thin film model catalysts:: Infrared study of CO adsorption [J].
Bertarione, S ;
Scarano, D ;
Zecchina, A ;
Johánek, V ;
Hoffmann, J ;
Schauermann, S ;
Frank, MM ;
Libuda, J ;
Rupprechter, G ;
Freund, HJ .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (11) :3603-3613
[5]   Water-Gas Shift and Formaldehyde Reforming Activity Determined by Defect Chemistry of Polycrystalline In2O3 [J].
Bielz, T. ;
Lorenz, H. ;
Amann, P. ;
Kloetzer, B. ;
Penner, S. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (14) :6622-6628
[6]   Hydrogen on In2O3: Reducibility, Bonding, Defect Formation, and Reactivity [J].
Bielz, Thomas ;
Lorenz, Harald ;
Jochum, Wilfrid ;
Kaindl, Reinhard ;
Klauser, Frederik ;
Kloetzer, Bernhard ;
Penner, Simon .
JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (19) :9022-9029
[7]   PROMOTION OF CO AND CO2 HYDROGENATION OVER RH BY METAL-OXIDES - THE INFLUENCE OF OXIDE LEWIS ACIDITY AND REDUCIBILITY [J].
BOFFA, A ;
LIN, C ;
BELL, AT ;
SOMORJAI, GA .
JOURNAL OF CATALYSIS, 1994, 149 (01) :149-158
[8]   Characterization by CO/FTIR spectroscopy of Pd/silica catalysts and its correlation with syn-gas conversion [J].
Cabilla, GC ;
Bonivardi, AL ;
Baltanás, MA .
CATALYSIS LETTERS, 1998, 55 (3-4) :147-156
[9]   CH3O decomposition on PdZn(111), Pd(111), and Cu(111).: A theoretical study [J].
Chen, ZX ;
Neyman, KM ;
Lim, KH ;
Rösch, N .
LANGMUIR, 2004, 20 (19) :8068-8077
[10]   THE CHEMISORPTION OF CO ON PD(110) AT 110 AND 300-K STUDIED BY ELECTRON-ENERGY LOSS SPECTROSCOPY [J].
CHESTERS, MA ;
MCDOUGALL, GS ;
PEMBLE, ME ;
SHEPPARD, N .
SURFACE SCIENCE, 1985, 164 (2-3) :425-436