水团簇构象稳定性起源和本质的密度泛函理论与量子分子动力学研究

doi:10.3866/PKU.WHXB201308272

物理化学学报 >> 2013, Vol. 29 >> Issue (10): 2173-2179.doi: 10.3866/PKU.WHXB201308272

水团簇构象稳定性起源和本质的密度泛函理论与量子分子动力学研究

王友娟¹, 赵东波¹, 荣春英¹, 刘述斌^1,2

1 湖南师范大学化学化工学院, 资源精细化与先进材料湖南省高校重点实验室, 化学生物学及中药分析教育部重点实验室, 长沙 410081;
2 Research Computing Center, University of North Carolina, Chapel Hill, North Carolina 27599-3420, U.S.A.

收稿日期:2013-06-27 修回日期:2013-08-27 发布日期:2013-09-26
通讯作者: 荣春英, 刘述斌 E-mail:rongchunying@aliyun.com;shubin@email.unc.edu
基金资助:
湖南师范大学“潇湘学者”杰出人才项目(23040609);湖南省研究生创新项目(CX2012B223)以及湖南省高等教育机构科技创新研究团队项目资助

Towards Understanding the Origin and Nature of the Conformational Stability of Water Clusters：a Density Functional Theory and Quantum Molecular Dynamics Study

WANG You-Juan¹, ZHAO Dong-Bo¹, RONG Chun-Ying¹, LIU Shu-Bin^1,2

1 Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research (Ministry of Education of China) and Key Laboratory of Resource Fine-Processing and Advanced Materials of Hunan Province, College of Chemistry and Chemical Engineering, Hunan Normal University, Changsha 410081, P. R. China;
2 Research Computing Center, University of North Carolina, Chapel Hill, North Carolina 27599-3420, U.S.A.

Received:2013-06-27 Revised:2013-08-27 Published:2013-09-26
Contact: RONG Chun-Ying, LIU Shu-Bin E-mail:rongchunying@aliyun.com;shubin@email.unc.edu
Supported by:
The project was supported by the‘XiaoXiang Scholar’Talents Foundation of Hunan Normal University, China (23040609), Hunan Provincial Innovation Foundation for Postgraduate, China (CX2012B223), and Aid Programfor Science and Technology Innovative Research Team in Higher Educational Institutions of Hunan Province, China.

摘要/Abstract

摘要：

寻找确定分子体系构象稳定性的关键因素是至关重要的, 但即使对最简单的分子, 其稳定性的起源和本质仍存在很大的争议. 本文以水团簇为例, 采用量子分子动力学产生185个八聚水分子团簇模型, 并运用基于密度泛函理论的两个能量分解方法寻找其稳定性的决定因素. 我们发现不同水团簇的稳定性与其立体排斥能和交换相关能成良好的线性关系.本文还采用双变量模型模拟水团簇的稳定性, 取得了更好的结果(相关系数大于0.99). 本工作对揭示包括水分子团簇在内的通过弱相互作用组成的分子络合物的稳定性起源和本质提供了有益启示.

关键词: 水分子团簇, 量子分子动力学, 密度泛函理论, 立体效应, 交换相关能

Abstract:

To find out what interaction dictates the molecular stability is essential, yet still controversial even for simplest molecules. Here, using water cluster as an example, we employ quantum molecular dynamics to generate a total of 185 conformations for octamer water clusters and then employ two energy partition schemes from density functional theory to pinpoint the principles governing their stability. We found that their stability is strongly correlated with steric repulsion and exchange-correlation interactions. Explanations using two different quantities are also proposed (with the correlation coefficient larger than 0.99). This work sheds light to the fundamental understanding towards the origin and nature of molecular conformational stability for water clusters and other molecular complexes formed through intermolecular interactions.

Key words: Water cluster, Quantum molecular dynamics, Density functional theory, Steric effect, Exchange-correlation energy

MSC2000:

O641

王友娟, 赵东波, 荣春英, 刘述斌. 水团簇构象稳定性起源和本质的密度泛函理论与量子分子动力学研究[J]. 物理化学学报, 2013, 29(10): 2173-2179.

WANG You-Juan, ZHAO Dong-Bo, RONG Chun-Ying, LIU Shu-Bin. Towards Understanding the Origin and Nature of the Conformational Stability of Water Clusters：a Density Functional Theory and Quantum Molecular Dynamics Study[J]. Acta Phys. -Chim. Sin., 2013, 29(10): 2173-2179.

参考文献

(1) Liu, S. B. J. Phys. Chem. A 2013, 117, 962. doi: 10.1021/jp312521z
(2) Pophristic, V.; Goodman, L. Nature 2001, 411, 565. doi: 10.1038/35079036
(3) Bickelhaupt, F. M.; Baerends, E. J. Angew. Chem. Int. Edit.2003, 42, 4183.
(4) Weinhold, F. Angew. Chem. Int. Edit. 2003, 42, 4188.
(5) Mo, Y. R. Nat. Chem. 2010, 2, 666. doi: 10.1038/nchem.721
(6) Mo, Y.; Gao, J. Accounts Chem. Res. 2007, 40, 113. doi: 10.1021/ar068073w
(7) Parr, R. G.; Yang, W. Density Functional Theory of Atoms Molecules; Oxford University Press: NewYork, 1989.
(8) Geerlings, P.; De Proft, F.; Langenaeker, W. Chem. Rev. 2003,103, 1793. doi: 10.1021/cr990029p
(9) Liu, S. B. Acta Phys. -Chim. Sin. 2009, 25, 590. [刘述斌. 物理化学学报, 2009, 25, 590.] doi: 10.3866/PKU.WHXB20090332
(10) Levy, M.; Perdew, J. P. Phys. Rev. A 1985, 32, 2010. doi: 10.1103/PhysRevA.32.2010
(11) Liu, S. B.; Parr, R. G. Phys. Rev. A 1996, 53, 2211. doi: 10.1103/PhysRevA.53.2211
(12) Liu, S. B.; Nagy, A.; Parr, R. G. Phys. Rev. A 1999, 59, 1131.doi: 10.1103/PhysRevA.59.1131
(13) Liu, S. B.; Morrison, R. C.; Parr, R. G. J. Chem. Phys. 2006,125, 174109. doi: 10.1063/1.2378769
(14) Liu, S. B. J. Chem. Phys. 2007, 126, 244103. doi: 10.1063/1.2747247
(15) March, N. H. Phys. Lett. A 1986, 113, 476. doi: 10.1016/0375-9601(86)90123-4
(16) Holas, A.; March, N. H. Phys. Rev. A 1991, 44, 5521. doi: 10.1103/PhysRevA.44.5521
(17) von Weizsäcker, C. F. Z. Phys. 1935, 96, 431. doi: 10.1007/BF01337700
(18) Weisskopf, V. F. Science 1975, 187, 605. doi: 10.1126/science.187.4177.605
(19) Liu, S. B. Phys. Rev. A 1996, 54, 4863. doi: 10.1103/PhysRevA.54.4863
(20) Liu, S. B.; Parr, R. G. Phys. Rev. A 1997, 55, 1792. doi: 10.1103/PhysRevA.55.1792
(21) Tsirelson, V. G.; Stash, A. I.; Liu, S. B. J. Chem. Phys. 2010,133, 114110. doi: 10.1063/1.3492377
(22) Liu, S. B. J. Chem. Phys. 2007, 126, 191107. doi: 10.1063/1.2741244
(23) Esquivel, R. O.; Liu, S. B.; Angulo, J. C.; Dehesa, J. S.; Antolín,J.; Molina-Espíritu, M. J. Phys. Chem. A 2011, 115, 4406. doi: 10.1021/jp1095272
(24) Liu, S. B.; Govind, N. J. Phys. Chem. A 2008, 112, 6690. doi: 10.1021/jp800376a
(25) Liu, S. B.; Govind, N.; Pedersen, L. G. J. Chem. Phys. 2008,129, 094104. doi: 10.1063/1.2976767
(26) Liu, S. B.; Hu, H.; Pedersen, L. G. J. Phys. Chem. A 2010, 114,5913. doi: 10.1021/jp101329f
(27) Ess, D. H.; Liu, S. B.; De Proft, F. J. Phys. Chem. A 2010, 114,12952. doi: 10.1021/jp108577g
(28) Huang, Y.; Zhong, A. G.; Yang, Q.; Liu, S. B. J. Chem. Phys.2011, 134, 084103. doi: 10.1063/1.3555760
(29) Zhao, D. B.; Rong, C. Y.; Jenkins, S.; Kirk, S. R.; Yin, D. L.;Liu, S. B. Acta Phys. -Chim. Sin. 2013, 29, 43. [赵东波, 荣春英,苏曼,苏文,尹笃林, 刘述斌.物理化学学报, 2013, 29,43.] doi: 10.3866/PKU.WHXB201211121
(30) Tsirelson, V. G.; Stash, A. I.; Karasiev, V. V.; Liu, S. B. Comp. Theor. Chem. 2013, 1006, 92. doi: 10.1016/j.comptc.2012.11.015
(31) Torrent-Sucarrat, M.; Liu, S. B.; De Proft, F. J. Phys. Chem. A2009, 113, 3698. doi: 10.1021/jp8096583
(32) Liu, S. B. J. Chem. Sci. 2005, 117, 477; Zhong, A. G.; Rong, C.Y.; Liu, S. B. J. Phys. Chem. A 2007, 111, 3132. doi: 10.1007/BF02708352
(33) Valiev, M.; Bylaska, E. J.; Govind, N.; Kowalski, K.; Straatsma,T. P.; Van Dam, H. J. J.; Wang, D.; Nieplocha, J.; Apra, E.;Windus, T. L.; de Jong, W. Comput. Phys. Commun. 2010, 181,1477.
(34) Maeda, S.; Ohno, K. J. Phys. Chem. A 2007, 111, 4527. doi: 10.1021/jp070606a
(35) Zhao, Y.; Truhlar, D. G. Theor. Chem. Acc. 2008, 120, 215. doi: 10.1007/s00214-007-0310-x
(36) Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; et al . Gaussian 09,Revision C. 01; Gaussian, Inc.: Wallingford, CT, 2009.
(37) Kitaura, K.; Morokuma, K. Int. J. Quantum Chem. 1976, 10,325.

[1]	李诗涵,赵侦超,李世坤,邢友东,张维萍. DFT计算结合固体NMR研究富铝SSZ-13的铝分布和Brønsted酸性[J]. 物理化学学报, 2020, 36(4): 1903021 -0 .
[2]	黄智超,戴亚中,温晓杰,刘丹,林宇轩,徐珍,裴坚,吴凯. Au(111)表面Verdazyl自由基的构象转换[J]. 物理化学学报, 2020, 36(1): 1907043 -0 .
[3]	王丹,丁迅雷,廖珩璐,戴佳钰. 单个金或银原子掺杂的氧化钒团簇上的甲烷活化反应[J]. 物理化学学报, 2019, 35(9): 1005 -1013 .
[4]	陈强,姜利学,李海方,陈娇娇,赵艳霞,何圣贵. 钒硼双原子阳离子活化甲烷研究[J]. 物理化学学报, 2019, 35(9): 1014 -1020 .
[5]	韩萌茹,周亚男,周旋,储伟. 通过g-C₃N₄担载MNi₁₂ (Fe, Co, Cu, Zn)纳米团簇调节甲烷化[J]. 物理化学学报, 2019, 35(8): 850 -857 .
[6]	赵越,崔佳桐,胡继闯,马嘉璧. VO_1-4⁺阳离子与n-C_mH_2m+2 (m = 3, 5, 7)烷烃的反应性研究：氧含量和碳链长度的影响[J]. 物理化学学报, 2019, 35(5): 531 -538 .
[7]	许文武,高嶷. 巯基保护的中空金纳米球[J]. 物理化学学报, 2018, 34(7): 770 -775 .
[8]	卢天,陈沁雪. 通过价层电子密度分析展现分子电子结构[J]. 物理化学学报, 2018, 34(5): 503 -513 .
[9]	尹玥琪,蒋梦绪,刘春光. Keggin型多酸负载的单原子催化剂(M₁/POM, M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW₁₂O₄₀]^3-)活化氮气分子的密度泛函理论计算研究[J]. 物理化学学报, 2018, 34(3): 270 -277 .
[10]	尹凡华,谭凯. 符合独立五元环规则的C₁₀₀(417)Cl₂₈形成机理的密度泛函理论研究[J]. 物理化学学报, 2018, 34(3): 256 -262 .
[11]	钟爱国,李嵘嵘,洪琴,张杰,陈丹. 从能量和信息理论视角理解单取代烷烃的异构化[J]. 物理化学学报, 2018, 34(3): 303 -313 .
[12]	丁晓琴,丁俊杰,李大禹,潘里,裴承新. 基于概念密度泛函理论磷酸酯类反应性物质毒性预测[J]. 物理化学学报, 2018, 34(3): 314 -322 .
[13]	王心怡,谢磊,丁元琪,姚心仪,张弛,孔惠慧,王利坤,许维. 超高真空条件下碱基与金属在Au(111)表面的相互作用[J]. 物理化学学报, 2018, 34(12): 1321 -1333 .
[14]	陈驰,张雪,周志有,张新胜,孙世刚. S掺杂促进Fe/N/C催化剂氧还原活性的实验与理论研究[J]. 物理化学学报, 2017, 33(9): 1875 -1883 .
[15]	刘玉玉,李杰伟,薄一凡,杨磊,张效霏,解令海,仪明东,黄维. 芴基张力半导体结构和光电性质的理论研究[J]. 物理化学学报, 2017, 33(9): 1803 -1810 .

水团簇构象稳定性起源和本质的密度泛函理论与量子分子动力学研究

Towards Understanding the Origin and Nature of the Conformational Stability of Water Clusters：a Density Functional Theory and Quantum Molecular Dynamics Study

PDF (PC)

赞

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

Metrics

本文评价

推荐阅读 0