Size-Dependent Sulfur Poisoning of Silica-Supported Monodisperse Pt Nanoparticle Hydrogenation Catalysts

被引:32
作者
Baldyga, Lyndsey M. [1 ]
Blavo, Selasi O. [1 ]
Kuo, Chun-Hong [2 ]
Tsung, Chia-Kuang [2 ]
Kuhn, John N. [1 ]
机构
[1] Univ S Florida, Dept Chem & Biomed Engn, Tampa, FL 33620 USA
[2] Boston Coll, Dept Chem, Chestnut Hill, MA 02467 USA
来源
ACS CATALYSIS | 2012年 / 2卷 / 12期
关键词
platinum; sulfur poisoning; colloidal synthesis with size control; structure sensitivity; ELECTRON-BEAM LITHOGRAPHY; ETHYLENE HYDROGENATION; PARTICLE-SIZE; PLATINUM NANOPARTICLES; BENZENE HYDROGENATION; STRUCTURE SENSITIVITY; HYDRODESULFURIZATION; 4,6-DIMETHYLDIBENZOTHIOPHENE; SBA-15; PD;
D O I
10.1021/cs300625m
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
Colloidal techniques were used to synthesize monodisperse Pt nanoparticles of four distinct sizes between 2 and 7 nm before immobilization onto silica. Ethylene hydrogenation demonstrated structure-insensitive behavior with TOFs of similar to 12 s(-1) before poisoning. With thiophene being a strong binding adsorbate, TOFs decreased by orders of magnitude, and the poisoning-induced antipathetic structure sensitivity because thiophene adsorbed more strongly to the coordinatively unsaturated, as compared with coordinatively saturated, surfaces, and the degree of saturation increased with decreasing Pt size. This effort is part of a broader study in which structure sensitivity is analyzed for adsorbates in complex reaction networks.
引用
收藏
页码:2626 / 2629
页数:4
相关论文
共 40 条
[1]  
[Anonymous], J ASTM INT
[2]   ETHYLENE HYDROGENATION ON PT(111) AND (5X20)PT(100) NEAR ATMOSPHERIC-PRESSURE [J].
BACKMAN, AL ;
MASEL, RI .
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A-VACUUM SURFACES AND FILMS, 1988, 6 (03) :1137-1139
[3]  
Bartholomew CH, 2006, FUNDAMENTALS OF INDUSTRIAL CATALYTIC PROCESSES, 2ND EDITION, P1, DOI 10.1002/9780471730071
[4]   Platinum nanoparticle shape effects on benzene hydrogenation selectivity [J].
Bratlie, Kaitlin M. ;
Lee, Hyunjoo ;
Komvopoulos, Kyriakos ;
Yang, Peidong ;
Somorjai, Gabor A. .
NANO LETTERS, 2007, 7 (10) :3097-3101
[5]   Sum frequency generation vibrational spectroscopic and high-pressure scanning tunneling microscopic studies of benzene hydrogenation on Pt(111) [J].
Bratlie, Kaitlin M. ;
Montano, Max O. ;
Flores, Lucio D. ;
Paajanen, Matti ;
Somorjai, Gabor A. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (39) :12810-12816
[6]   Deep desulfurization:: reactions, catalysts and technological challenges [J].
Breysse, M ;
Djega-Mariadassou, G ;
Pessayre, S ;
Geantet, C ;
Vrinat, M ;
Pérot, G ;
Lemaire, M .
CATALYSIS TODAY, 2003, 84 (3-4) :129-138
[7]   Overview of support effects in hydrotreating catalysts [J].
Breysse, M ;
Afanasiev, P ;
Geantet, C ;
Vrinat, M .
CATALYSIS TODAY, 2003, 86 (1-4) :5-16
[8]   THE INFLUENCE OF PARTICLE-SIZE ON THE CATALYTIC PROPERTIES OF SUPPORTED METALS [J].
CHE, M ;
BENNETT, CO .
ADVANCES IN CATALYSIS, 1989, 36 :55-172
[9]   Fabrication of platinum nanoparticles and nanowires by electron beam lithography (EBL) and nanoimprint lithography (NIL): comparison of ethylene hydrogenation kinetics [J].
Contreras, AM ;
Grunes, J ;
Yan, XM ;
Liddle, A ;
Somorjai, GA .
CATALYSIS LETTERS, 2005, 100 (3-4) :115-124
[10]   Aromatic saturation of distillates: An overview [J].
Cooper, BH ;
Donnis, BBL .
APPLIED CATALYSIS A-GENERAL, 1996, 137 (02) :203-223