Optimisation of preparation method for Pd doped Cu/Al2O3 catalysts for selective acetylene hydrogenation

被引:90
作者
McCue, Alan J. [1 ]
Shepherd, Ashley M. [2 ]
Anderson, James A. [1 ,3 ]
机构
[1] Univ Aberdeen, Dept Chem, Surface Chem & Catalysis Grp, Aberdeen AB24 3UE, Scotland
[2] Univ Oxford, Chem Res Lab, Oxford OX1 3TA, England
[3] Univ Aberdeen, Sch Engn, Mat & Chem Engn Grp, Aberdeen AB24 3UE, Scotland
关键词
GALLIUM INTERMETALLIC COMPOUNDS; ION-EXCHANGED COPPER; PALLADIUM CATALYSTS; SUBSURFACE CARBON; PROPYNE; NANOPARTICLES; ETHYLENE; SITES; MONOXIDE; ALKYNES;
D O I
10.1039/c5cy00253b
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Pd doped Cu catalysts have been prepared by co-impregnation, sequential impregnation and a colloidal approach. In each case, the Cu : Pd ratio was optimised leading to catalyst activity which exceeded that offered by monometallic Cu at low temperature (393 K and below) but with a product selectivity which suggests the reaction is still taking place on a Cu surface (i.e., high ethylene selectivity). Pd is therefore thought to influence hydrogen dissociation rates and enhance spillover onto Cu sites. Catalytic testing under more demanding conditions showed differences between the preparation methods. In general, the most active of the samples appeared to be the least selective and vice-versa. Under optimised conditions, a 50: 1 Cu: Pd ratio prepared by sequential impregnation showed an ethylene selectivity of 80% at 98% conversion at only 353 K. Further testing under competitive conditions suggested good ethylene selectivity could be retained under industrially relevant conditions in the absence of CO.
引用
收藏
页码:2880 / 2890
页数:11
相关论文
共 55 条
[1]   Activated takovite catalysts for partial hydrogenation of ethyne, propyne, and propadiene [J].
Abello, Sonia ;
Verboekend, Danny ;
Bridier, Blaise ;
Perez-Ramirez, Javier .
JOURNAL OF CATALYSIS, 2008, 259 (01) :85-95
[2]   Impact of Organic Ligands on the Structure and Hydrogenation Performance of Colloidally Prepared Bimetallic PtSn Nanoparticles [J].
Altmann, Lena ;
Wang, Xiaodong ;
Stoever, Joerg ;
Klink, Miriam ;
Zielasek, Volkmar ;
Thiel, Karsten ;
Kolny-Olesiak, Joanna ;
Al-Shamery, Katharina ;
Borchert, Holger ;
Parisi, Juergen ;
Baeumer, Marcus .
CHEMCATCHEM, 2013, 5 (07) :1803-1810
[3]   How to Control the Selectivity of Palladium-based Catalysts in Hydrogenation Reactions: The Role of Subsurface Chemistry [J].
Armbruester, Marc ;
Behrens, Malte ;
Cinquini, Fabrizio ;
Foettinger, Karin ;
Grin, Yuri ;
Haghofer, Andreas ;
Kloetzer, Bernhard ;
Knop-Gericke, Axel ;
Lorenz, Harald ;
Ota, Antje ;
Penner, Simon ;
Prinz, Jan ;
Rameshan, Christoph ;
Revay, Zsolt ;
Rosenthal, Dirk ;
Rupprechter, Nther ;
Sautet, Philippe ;
Schloegl, Robert ;
Shao, Lidong ;
Szentmiklosi, Laszlo ;
Teschner, Detre ;
Torres, Daniel ;
Wagner, Ronald ;
Widmer, Roland ;
Wowsnick, Gregor .
CHEMCATCHEM, 2012, 4 (08) :1048-1063
[4]   Formation of polymer-grade ethylene by selective hydrogenation of acetylene over Au/CeO2 catalyst [J].
Azizi, Yassine ;
Petit, Corinne ;
Pitchon, Veronique .
JOURNAL OF CATALYSIS, 2008, 256 (02) :338-344
[5]  
Bastista J., 2001, APPL CATAL A-GEN, V206, P113
[6]   Selective hydrogenation of ethyne in ethene-rich streams on palladium catalysts, Part 2: Steady-state kinetics and effects of palladium particle size, carbon monoxide, and promoters [J].
Borodzinski, Andrzej ;
Bond, Geoffrey C. .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2008, 50 (03) :379-469
[7]   Single atom alloy surface analogs in Pd0.18Cu15 nanoparticles for selective hydrogenation reactions [J].
Boucher, Matthew B. ;
Zugic, Branko ;
Cladaras, George ;
Kammert, James ;
Marcinkowski, Matthew D. ;
Lawton, Timothy J. ;
Sykes, E. Charles H. ;
Flytzani-Stephanopoulos, Maria .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2013, 15 (29) :12187-12196
[8]   Permanent alkene selectivity enhancement in copper-catalyzed propyne hydrogenation by temporary CO supply [J].
Bridier, Blaise ;
Hevia, Miguel A. G. ;
Lopez, Nuria ;
Perez-Ramirez, Javier .
JOURNAL OF CATALYSIS, 2011, 278 (01) :167-172
[9]   Molecular understanding of alkyne hydrogenation for the design of selective catalysts [J].
Bridier, Blaise ;
Lopez, Nuria ;
Perez-Ramirez, Javier .
DALTON TRANSACTIONS, 2010, 39 (36) :8412-8419
[10]   Cooperative Effects in Ternary Cu-Ni-Fe Catalysts Lead to Enhanced Alkene Selectivity in Alkyne Hydrogenation [J].
Bridier, Blaise ;
Perez-Ramirez, Javier .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (12) :4321-4327