NH3 adsorption and dissociation on a nanosized iron cluster

被引：56

作者：

Lanzani, G. ^{[1
,2
]}

Laasonen, K. ^{[1
]}

机构：

[1] Univ Oulu, Dept Chem, Oulu 90014, Finland

[2] Univ Oulu, Thule Inst, Oulu 90014, Finland

来源：

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY | 2010年 / 35卷 / 13期

关键词：

DFT calculations; Molecular adsorption; Reaction kinetics; Ammonia decomposition; Nanosized iron catalyst; AMMONIA DECOMPOSITION; ULTRASOFT PSEUDOPOTENTIALS; CATALYTIC DECOMPOSITION; HYDROGEN-PRODUCTION; CO DISSOCIATION; METAL-CLUSTERS; KINETICS; NANOPARTICLES; GENERATION; PARTICLES;

D O I：

10.1016/j.ijhydene.2010.03.142

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：

We employed spin-polarized density functional theory to study the bonding and dissociation of NH3 and its fragment on a nanosized icosahedral Fe-55 cluster. The site-preference investigations, suggest that for NH3, only the interaction perpendicular to the cluster is favorable (-0.37 eV < B.E.(NH3) < +0.05 eV). Stable geometries of N and H on the high symmetry adsorption site of Fe-55 have been calculated as well. Both of these atoms have similar behavior: only the hollow or top sites are stable. Possible dissociation paths of the NH3 to atomic nitrogen and hydrogen were identified. The calculated lowest reaction barrier for the overall process is 1.48 eV. The rate limiting step is the first hydrogen removal from the NH3. Our results suggest that the catalytic activity of iron surfaces towards ammonia-like molecules is enhanched when the metal is in the nanostructured phase. (C) 2010 Professor T. Nejat Veziroglu. Published by Elsevier Ltd. All rights reserved.

引用

页码：6571 / 6577

页数：7

共 59 条

[1]

Aika K.-i., 1995, Ammonia: Catalysis and Manufacture

[2] Study of the ammonia decomposition over iron catalysts [J].

Arabczyk, W ;

Zamlynny, J .

CATALYSIS LETTERS, 1999, 60 (03) :167-171

[3]

ARABCZYK W, 1995, ADV MAT TECHNOL GLIW, V21

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

BLOCHL, PE .

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

[5] Why the optimal ammonia synthesis catalyst is not the optimal ammonia decomposition catalyst [J].

Boisen, A ;

Dahl, S ;

Norskov, JK ;

Christensen, CH .

JOURNAL OF CATALYSIS, 2005, 230 (02) :309-312

[6] PREPARATION, CHARACTERIZATION, AND APPLICATION OF FINE METAL PARTICLES AND METAL COLLOIDS USING HYDROTRIORGANOBORATES [J].

BONNEMANN, H ;

BRIJOUX, W ;

BRINKMANN, R ;

FRETZEN, R ;

JOUSSEN, T ;

KOPPLER, R ;

KORALL, B ;

NEITELER, P ;

RICHTER, J .

JOURNAL OF MOLECULAR CATALYSIS, 1994, 86 (1-3) :129-177

[7] Kinetics of NH3 decomposition over well dispersed Ru [J].

Bradford, MCJ ;

Fanning, PE ;

Vannice, MA .

JOURNAL OF CATALYSIS, 1997, 172 (02) :479-484

[8] The active site in nanopaticle gold catalysis [J].

Campbell, CT .

SCIENCE, 2004, 306 (5694) :234-235

[9] Numerical modeling of hydrogen production from ammonia decomposition for fuel cell applications [J].

Chein, Rei-Yu ;

Chen, Yen-Cho ;

Chang, Chia-San ;

Chung, J. N. .

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2010, 35 (02) :589-597

[10] Ammonia decomposition kinetics over Ni-Pt/Al2O3 for PEM fuel cell applications [J].

Chellappa, AS ;

Fischer, CM ;

Thomson, WJ .

APPLIED CATALYSIS A-GENERAL, 2002, 227 (1-2) :231-240

← 1 2 3 4 5 6 →