Descriptor-Based Analysis Applied to HCN Synthesis from NH3 and CH4

被引：70

作者：

Grabow, Lars C. ^{[1
]}

Studt, Felix ^{[2
]}

Abild-Pedersen, Frank ^{[2
]}

Petzold, Vivien ^{[3
]}

Kleis, Jesper ^{[3
]}

Bligaard, Thomas ^{[3
]}

Norskov, Jens K. ^{[1
,2
]}

机构：

[1] Stanford Univ, Dept Chem Engn, Stanford, CA 94305 USA

[2] SUNCAT Ctr Interface Sci & Catalysis, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA

[3] Tech Univ Denmark, Dept Phys, Ctr Atom Scale Mat Design, DK-2800 Lyngby, Denmark

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2011年 / 50卷 / 20期

关键词：

HCN synthesis; heterogeneous catalysis; reaction mechanisms; scaling relations; transition metals; SURFACE-CHEMISTRY; ALLOY CATALYSTS; METHANE; IDENTIFICATION; HYDROGENATION; ENERGIES; SELECTIVITY; REACTIVITY; EVOLUTION; PT(111);

D O I：

10.1002/anie.201100353

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

A trendy volcano: By the example of HCN synthesis from NH3 and CH4, it is demonstrated how scaling relations for intermediates and transition states provide a basis for the prediction of trends in heterogeneous catalysis (see logarithmic turnover frequency, TOF). These trends include not only the activity but also selectivity and the dominant reaction mechanism. This general approach can be applied to a large number of catalytic systems. © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

引用

页码：4601 / 4605

页数：5

共 43 条

[1] Scaling properties of adsorption energies for hydrogen-containing molecules on transition-metal surfaces [J].

Abild-Pedersen, F. ;

Greeley, J. ;

Studt, F. ;

Rossmeisl, J. ;

Munter, T. R. ;

Moses, P. G. ;

Skulason, E. ;

Bligaard, T. ;

Norskov, J. K. .

PHYSICAL REVIEW LETTERS, 2007, 99 (01)

[2] Toward computational screening in heterogeneous catalysis: Pareto-optimal methanation catalysts [J].

Andersson, MP ;

Bligaard, T ;

Kustov, A ;

Larsen, KE ;

Greeley, J ;

Johannessen, T ;

Christensen, CH ;

Norskov, JK .

JOURNAL OF CATALYSIS, 2006, 239 (02) :501-506

[3]

Andrussow L., 1955, CHEM-ING-TECH, V27, P469

[4] 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

[5] Micro- and macro-kinetics: their relationship in heterogeneous catalysis [J].

Campbell, Charles T. .

TOPICS IN CATALYSIS, 1994, 1 (3-4) :353-366

[6] SCANNING TUNNELING MICROSCOPY OF PLATINUM-RHODIUM GAUZE HCN CATALYSTS [J].

COWANS, BA ;

JURMAN, KA ;

DELGASS, WN ;

LI, YZ ;

REIFENBERGER, R ;

KOCH, TA .

JOURNAL OF CATALYSIS, 1990, 125 (02) :501-513

[7] HCN synthesis from methane and ammonia over platinum [J].

Delagrange, S. ;

Schuurman, Y. .

CATALYSIS TODAY, 2007, 121 (3-4) :204-209

[8] HCN synthesis from methane and ammonia:: mechanisms of Pt+-mediated C-N coupling [J].

Diefenbach, M ;

Brönstrup, M ;

Aschi, M ;

Schröder, D ;

Schwarz, H .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1999, 121 (45) :10614-10625

[9]

Fernandez EM, 2008, ANGEW CHEM, V120, P4761, DOI [10.1002/ange.200705739, DOI 10.1002/ANGE.200705739]

[10] Scaling relationships for adsorption energies on transition metal oxide, sulfide, and nitride surfaces [J].

Fernandez, Eva M. ;

Moses, Poul G. ;

Toftelund, Anja ;

Hansen, Heine A. ;

Martinez, Jose I. ;

Abild-Pedersen, Frank ;

Kleis, Jesper ;

Hinnemann, Berit ;

Rossmeisl, Jan ;

Bligaard, Thomas ;

Norskov, Jens K. .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2008, 47 (25) :4683-4686

← 1 2 3 4 5 →