Catalytic reduction of N2O by CO over PtlAum- clusters:A first-principles study

doi:10.1088/1674-1056/24/9/098201

中国物理B ›› 2015, Vol. 24 ›› Issue (9): 98201-098201.doi: 10.1088/1674-1056/24/9/098201

• INTERDISCIPLINARY PHYSICS AND RELATED AREAS OF SCIENCE AND TECHNOLOGY • 上一篇下一篇

Catalytic reduction of N₂O by CO over Pt_lAu_m^- clusters:A first-principles study

米鸿^a, 韦世豪^a, 段香梅^b, 潘孝胤^b

a Department of Microelectronic Science and Engineering, Faculty of Science, Ningbo University, Ningbo 315211, China;
b Department of Physics, Faculty of Science, Ningbo University, Ningbo 315211, China

收稿日期:2015-04-08 修回日期:2015-05-27 出版日期:2015-09-05 发布日期:2015-09-05
基金资助:
Project supported by the National Natural Science Foundation of China (Grants Nos. 10804058, 11174164, and 11275100), the Science Foundation of Zhejiang Province, China (Grant No. Y607546), and the K. C. Wong Magna Foundation in Ningbo University, China.

Catalytic reduction of N₂O by CO over Pt_lAu_m^- clusters:A first-principles study

Mi Hong (米鸿)^a, Wei Shi-Hao (韦世豪)^a, Duan Xiang-Mei (段香梅)^b, Pan Xiao-Yin (潘孝胤)^b

a Department of Microelectronic Science and Engineering, Faculty of Science, Ningbo University, Ningbo 315211, China;
b Department of Physics, Faculty of Science, Ningbo University, Ningbo 315211, China

Received:2015-04-08 Revised:2015-05-27 Online:2015-09-05 Published:2015-09-05
Contact: Wei Shi-Hao E-mail:weishihao@nbu.edu.cn
Supported by:
Project supported by the National Natural Science Foundation of China (Grants Nos. 10804058, 11174164, and 11275100), the Science Foundation of Zhejiang Province, China (Grant No. Y607546), and the K. C. Wong Magna Foundation in Ningbo University, China.

摘要/Abstract

摘要： Based on the density functional theory, we investigate negatively charged clusters Pt_lAu_m^- (l+m=4), which show significant catalytic properties in the simultaneous removal of N₂O and CO. We find that in these clusters, the platinum atom acts as the adsorption center for N₂O, the gold and Pt atoms act as electron donors during the reaction, and the charge transfers from the bimetallic cluster to the N₂O molecule. As the proportion of Au in the cluster increases, the d band center shifts down further away from the Fermi level, meanwhile more charge is transferred to the N₂O molecule, resulting in weaker N-O bond strength. Therefore bimetallic cluster PtAu₃^- shows better catalytic properties than the other clusters, especially pure Pt₄^- and Au₄^- clusters. This means that there is a synergetic effect between the Pt and Au atoms in the negatively charged bimetallic clusters. Our results help to reveal the mechanism of Pt_lAu_m^- bimetallic clusters as excellent catalysts.

关键词: bimetallic cluster, translate state, catalytic property, potential energy surface

Abstract: Based on the density functional theory, we investigate negatively charged clusters Pt_lAu_m^- (l+m=4), which show significant catalytic properties in the simultaneous removal of N₂O and CO. We find that in these clusters, the platinum atom acts as the adsorption center for N₂O, the gold and Pt atoms act as electron donors during the reaction, and the charge transfers from the bimetallic cluster to the N₂O molecule. As the proportion of Au in the cluster increases, the d band center shifts down further away from the Fermi level, meanwhile more charge is transferred to the N₂O molecule, resulting in weaker N-O bond strength. Therefore bimetallic cluster PtAu₃^- shows better catalytic properties than the other clusters, especially pure Pt₄^- and Au₄^- clusters. This means that there is a synergetic effect between the Pt and Au atoms in the negatively charged bimetallic clusters. Our results help to reveal the mechanism of Pt_lAu_m^- bimetallic clusters as excellent catalysts.

Key words: bimetallic cluster, translate state, catalytic property, potential energy surface

中图分类号: (Reactions on clusters)

82.33.Hk

36.40.Cg (Electronic and magnetic properties of clusters) 31.15.ve (Electron correlation calculations for atoms and ions: ground state)

米鸿, 韦世豪, 段香梅, 潘孝胤. Catalytic reduction of N₂O by CO over Pt_lAu_m^- clusters:A first-principles study[J]. 中国物理B, 2015, 24(9): 98201-098201.

Mi Hong (米鸿), Wei Shi-Hao (韦世豪), Duan Xiang-Mei (段香梅), Pan Xiao-Yin (潘孝胤). Catalytic reduction of N₂O by CO over Pt_lAu_m^- clusters:A first-principles study[J]. Chin. Phys. B, 2015, 24(9): 98201-098201.

参考文献 25

[1]	Ravishankara A R, Daniel J S and Portmann R W 2009 Science 326 123
[2]	Hamilton S M, Hopkins W S, Harding D J, Walsh T R, Haertelt M, Kerpal C, Gruene P, Meijer G, Fielicke A and Mackenzie S R 2011 J. Phys. Chem. A 115 2489
[3]	Chiodo S, Rondinelli F, Russo N and Toscano M 2008 J. Chem. Theory Comput. 4 316
[4]	Delabie A and Pierloot K 2002 J. Phys. Chem. A 106 5679
[5]	Wannakao S, Nongnual T, Khongpracha P, Maihom T and Limtrakul J 2012 J. Phys. Chem. C 116 16992
[6]	Blagojevic V, Orlova G and Bohme D K 2005 J. Am. Chem. Soc 127 3545
[7]	Ryan M F, Stoeckigt D and Schwarz H 1994 J. Am. Chem. Soc 116 9565
[8]	Michalak A, Witko M and Hermann K 1997 J. Mol. Catal. A: Chemical 119 213
[9]	Kappes M M and Staley R H 1981 J. Am. Chem. Soc 103 1286
[10]	Chen L L, Lu Q L and Luo Q Q 2010 Acta Phys. Sin. 59 234 (in Chinese)
[11]	Mao H P, Sheng Y and Wang H Y 2008 Chin. Phys. B 17 2110
[12]	Achatz U, Berg C, Joos S, Fox B S, Beyer M K, Niedner-Schatteburg G and Bondybey V E 2000 Chem. Phys. Lett. 320 53
[13]	Zhou M, Zhang A, Dai Z, Zhang C and Feng Y P 2010 J. Chem. Phys. 132 194704
[14]	Wang Y C, Wang Q Y, Geng Z Y, Si Y B, Zhang J H, Li H Z and Zhang Q L 2008 Chem. Phys. Lett. 460 13
[15]	Yamamoto H, Miyajima K and Yasuike T 2013 J. Phys. Chem. A 117 12175
[16]	Brönstrup M, Schröder D, Kretzschmar I, Schwarz H and Harvey J N 2001 J. Am. Chem. Soc 123 142
[17]	Balteanu I, Petru Balaj O, Beyer M K and Bondybey V E 2004 Phys. Chem. Chem. Phys. 6 2910
[18]	Siu C K, Reitmeier S J, Balteanu I, Bondybey V E and Beyer M K 2007 Eur. Phys. J. D 43 189
[19]	Wang F, Zhang D and Ding Y 2010 J. Phys. Chem. C 114 14076
[20]	Gao G P, Wei S H and Duan X M 2012 J. Phys. Chem. C 116 24930
[21]	Wang Y H, Zhu J L, Zhang J C, Song L F, Hu J Y, Ong S L and Ng W J 2006 J. Power Sources 155 440
[22]	Hammer B, Hansen L B and Norskov J K 1999 Phys. Rev. B 59 7413
[23]	Delley B 1990 J. Chem. Phys. 92 508
[24]	Delley B 2000 J. Chem. Phys. 113 7756
[25]	Chretien S, Gordon M S and Metiu H 2004 J. Chem. Phys. 121 3756

Catalytic reduction of N₂O by CO over Pt_lAu_m^- clusters:A first-principles study

Catalytic reduction of N₂O by CO over Pt_lAu_m^- clusters:A first-principles study

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