Single-Atom Alloy Pd-Ag Catalyst for Selective Hydrogenation of Acrolein

被引：170

作者：

Aich, Payoli ^{[1
]}

Wei, Haojuan ^{[1
]}

Basan, Bridget ^{[1
]}

Kropf, A. Jeremy ^{[2
]}

Schweitzer, Neil M. ^{[2
]}

Marshall, Christopher L. ^{[2
]}

Miller, Jeffrey T. ^{[2
,3
]}

Meyer, Randall ^{[1
]}

机构：

[1] Univ Illinois, Dept Chem Engn, Chicago, IL 60607 USA

[2] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA

[3] Purdue Univ, Sch Chem Engn, W Lafayette, IN 47907 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2015年 / 119卷 / 32期

基金：

美国国家科学基金会;

关键词：

TOTAL-ENERGY CALCULATIONS; HETEROGENEOUS CATALYSIS; SILVER; SENSITIVITY; REACTIVITY; ALDEHYDES; GAP;

D O I：

10.1021/acs.jpcc.5b01357

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-Ag alloy catalysts with very dilute amounts of Pd were synthesized. EXAFS results demonstrated that when the concentration of Pd was as low as 0.01 wt %, Pd was completely dispersed as isolated single atoms in Ag nanoparticles. The activity for the hydrogenation of acrolein was improved by the presence of these isolated Pd atoms due to the creation of sites with lower activation energy for H-2 dissociation. In addition, for the same particle size, the 0.01% Pd/8% Ag alloy nanoparticles exhibited higher selectivity than their monometallic counterparts, suggesting that the Pd atom may act as a site for the favorable bonding of the acrolein molecule for facile hydrogenation of the aldehyde functionality.

引用

收藏

页码：18140 / 18148

页数：9

相关论文

共 52 条

[1] An Atomic-Scale View of Palladium Alloys and their Ability to Dissociate Molecular Hydrogen [J].

Baber, Ashleigh E. ;

Tierney, Heather L. ;

Lawton, Timothy J. ;

Sykes, E. Charles H. .

CHEMCATCHEM, 2011, 3 (03) :607-614

[2] Surface chemistry and catalysis on well-defined oxide surfaces: nanoscale design bases for single-site heterogeneous catalysts [J].

Barteau, MA ;

Lyons, JE ;

Song, IK .

JOURNAL OF CATALYSIS, 2003, 216 (1-2) :236-245

[3] The Bronsted-Evans-Polanyi relation and the volcano curve in heterogeneous catalysis [J].

Bligaard, T ;

Norskov, JK ;

Dahl, S ;

Matthiesen, J ;

Christensen, CH ;

Sehested, J .

JOURNAL OF CATALYSIS, 2004, 224 (01) :206-217

[4] PROJECTOR AUGMENTED-WAVE METHOD [J].

BLOCHL, PE .

PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979

[5] 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

[6] Bridging the pressure and materials gap:: in-depth characterisation and reaction studies of silver-catalysed acrolein hydrogenation [J].

Bron, M ;

Teschner, D ;

Knop-Gericke, A ;

Steinhauer, B ;

Scheybal, A ;

Hävecker, M ;

Wang, D ;

Födisch, R ;

Hönicke, D ;

Wootsch, A ;

Schlögl, R ;

Claus, P .

JOURNAL OF CATALYSIS, 2005, 234 (01) :37-47

[7] Silver as acrolein hydrogenation catalyst:: intricate effects of catalyst nature and reactant partial pressures [J].

Bron, Michael ;

Teschner, Detre ;

Knop-Gericke, Axel ;

Jentoft, Friederike C. ;

Kroehnert, Jutta ;

Hohmeyer, Jens ;

Volckmar, Claudia ;

Steinhauer, Bernd ;

Schloegl, Robert ;

Claus, Peter .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2007, 9 (27) :3559-3569

[8] Homogeneous and heterogeneous catalysis:: Bridging the gap through surface organometallic chemistry [J].

Copéret, C ;

Chabanas, M ;

Saint-Arroman, RP ;

Basset, JM .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2003, 42 (02) :156-181

[9] Silica-bound homogenous catalysts as recoverable and reusable catalysts in organic synthesis [J].

Corma, Avelino ;

Garcia, Hermenegildo .

ADVANCED SYNTHESIS & CATALYSIS, 2006, 348 (12-13) :1391-1412

[10] Influence of Sn additives on the selectivity of hydrogenation of α-β-unsaturated aldehydes with Pt catalysts:: a density functional study of molecular adsorption [J].

Delbecq, F ;

Sautet, P .

JOURNAL OF CATALYSIS, 2003, 220 (01) :115-126

← 1 2 3 4 5 6 →