密度泛函理论研究Hg与Auqn(n=1—6, q=0,+1,-1) 团簇的相互作用

孙路石; 张安超; 向军; 郭培红; 刘志超; 苏胜

doi:10.7498/aps.60.073103

摘要

采用密度泛函理论中的广义梯度近似对Hg与小团簇Au qn (n=1—6, q=0, +1, -1)的相互作用进行了系统研究. 结果表明,除Au5+,-团簇外,前线分子轨道理论可以成功预测大部分Au n Hg q 复合物的最低能量结构. Aun团簇对Hg的吸附受团簇尺寸大小和团簇所携带电荷的影

关键词:

密度泛函理论 /
汞 /
金团簇 /
吸附能

Elemental mercury (Hg) adsorptions on small neutral, cationic and anionic gold clusters, Auqn (n=1—6, q=0, +1, -1), are systematically investigated by using the density functional theory(DFT) in the generalized gradient approximation. The result shows that the frontier molecular orbital theory (FMOT) is useful for predicting the favorable binding configurations of Hg adsorbed on neutral and charged Aun clusters. Most of the lowest energy AunHg complexes can be successfully predicted. The size and the charge state of the clusters have strong influence on the adsorption of Hg on gold clusters. The adsorption energy on the neutral clusters reaches a local maximum at n=4, which is about 0.661eV. The adsorption energies for cationic clusters decrease with cluster size increasing, although there is a local peak at n=5. Similarly, for anionic clusters, the adsorption energies decrease with cluster size, except for n=3. The adsorption energies on the cationic clusters are generally stronger than those on the neutral and anionic clusters. For the lowest energy AunHg complexes, an approximate linear correlation between the adsorption energy and the Mulliken charge on adsorbed Hg is found. The more the charges transfer to the cluster, the higher the adsorption energy is.

Keywords:

作者及机构信息

(1)河南理工大学机械与动力工程学院,焦作 454003; (2)华中科技大学煤燃烧国家重点实验室,武汉 430074; (3)华中科技大学煤燃烧国家重点实验室,武汉 430074;河南理工大学机械与动力工程学院,焦作 454003

基金项目: 国家重点基础研究发展计划项目(批准号:2010CB227003),国家自然科学基金(批准号:50976038)和河南省重点学科(批准号:507907)资助的课题.

Authors and contacts

(1)School of Mechanical and Power Enginneering, Henan Polytechnic University, Jiaozuo 454003, China; (2)State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China; (3)State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China;School of Mechanical and Power Enginneering, Henan Polytechnic University, Jiaozuo 454003, China

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施引文献

[1]	Ren J L,Zhou J S,Luo Z Y,Zhong Y J,Zhang X M 2006 Proceedings of the CSEE 26 1(in Chinese)[任建莉、周劲松、骆仲泱、钟英杰、张雪梅 2006 中国电机工程学报 26 1]
[2]	Zhou J S,Wang Y,Hu C X,He S,Luo Z Y,Ni M J,Cen K F 2008 Journal of Power Engineering 28 625(in Chinese)[周劲松、王岩、胡长兴、何胜、骆仲泱、倪明江、岑可法 2008 动力工程 28 625]
[3]	Guo X,Zheng C G,Jia X H,Lin Z,Liu Y N 2004 Proceedings of the CSEE 24 185(in Chinese)[郭欣、郑楚光、贾小红、林钊、刘亚男 2004 中国电机工程学报 24 185]
[4]	Yan T Y 1994 Ind. Eng. Chem. Res. 33 3010
[5]	Liu Y,Kelly D J A,Yang H Q,Lin C C H,Kuznicki S M,Xu Z H 2008 Envrion. Sci. Technol. 42 6205
[6]	Dong J,Xu Z H,Kuznicki S M 2009 Environ. Sci. Technol. 43 3266
[7]	Zhao Y X,Mann M,Pavlish J,Mieck B F,Dunham G,Olson E 2006 Environ. Sci. Technol. 40 1603
[8]	Poulston S,Granite E J,Pennline H W,Christina R,Myers C R, Stanko D P 2007 Fuel 86 2201
[9]	Sasmaz E,Aboud S,Wilcox J 2009 J. Phys. Chem. C 113 7813
[10]	Aboud S,Sasmaz E,Wilcox J 2008 Main Group Chemistry 7 205
[11]	Steckel J A 2008 Physical Review B 77 115412
[12]	Ding X L,Li Z Y,Yang J L,Hou J G,Zhu Q S 2004 J. Chem. Phys. 120 9594
[13]	Zhou J,Li Z H,Wang W N,Fan K N 2006 J. Phys. Chem. A 110 7167
[14]	Poater A,Duran M,Jaque P,Toro-Labbé A,Solà M 2006 J. Phys. Chem. B 110 6526
[15]	Kang G J,Chen Z X,Li Z,He X 2009 J. Chem. Phys. 130 034701
[16]	Ding X L,Li Z Y,Yang J L,Hou J G,Zhu Q S 2004 J. Chem. Phys. 121 2558
[17]	Ghebriel H W 2007 J. Chem. Phys. 126 244705
[18]	Chrétien S,Gordon H,Metiu H 2004 J. Chem. Phys. 121 9925
[19]	Chrétien S,Gordon H,Metiu H 2004 J. Chem. Phys. 121 3756
[20]	Mao H P,Wang H Y,Sheng Y 2008 Chin. Phys. B 17 2110
[21]	Deka A,Deka R C 2008 Journal of Molecular Structure: Theochem 870 83
[22]	Delly B 1990 J. Chem. Phys. 92 508
[23]	Delly B 2000 J. Chem. Phys. 113 7756
[24]	Elanany M,Koyama M,Kubo M,Selvam P,Miyamoto A 2004 Microporous and Mesoporous Materials 71 51
[25]	Jennifer W,Joe R,David C J,Marsden P B 2003 Environ. Sci. Technol. 37 4199
[26]	Peterson K A,Puzzarini C 2005 Theor. Chem. Acc. 114 283
[27]	Wesendrup R,Laerdahl J K,Schwerdtfegera P 1999 J. Chem. Phys. 110 9458
[28]	Li Q,Huang Y H,Chen G J 2008 Structural Chemistry(Beijing:Beijing Normal University Press)(in Chinese)[李奇、黄元河、陈光巨 2008 结构化学(北京: 北京师范大学出版社)]
[29]	Wells D H,Delgass W N,Thomsona K T 2002 J. Chem. Phys. 117 10597
[30]	Joshi A M, Delgass W N, Thomson K T. 2006 J. Phys. Chem. B 110 23373
[31]	Ge G X,Yang Z Q,Cao H B 2009 Acta Phys. Sin. 58 6128(in Chinese)[葛桂贤、杨增强、曹海滨 2009 物理学报58 6128]
[32]	Ge G X,Yang Z Q,Jing Q,Luo Y H 2009 Acta Phys. Sin. 58 8236(in Chinese)[葛桂贤、杨增强、井群、罗有华 2009 物理学报 58 8236]
[33]	Lei X L 2010 Chin. Phys. B 19 107103
[34]	Zhao W J,Lei X L,Yan Y L,Luo Y H 2007 Acta Phys. Sin. 56 5210(in Chinese)[赵文杰、雷雪玲、闫玉丽、杨致、罗有华 2007 物理学报 56 5210]
[35]	Fernández E M,Soler J M,Garzón I L,Balbás L C 2004 Physical Review B 70 165403

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