Theoretical Study on Realization of Nonequilibrium Reaction Field Analogs by Unique Aggregated Coordination Space
唯一聚合配位空间实现非平衡反应场类似物的理论研究
基本信息
- 批准号:16074207
- 负责人:
- 金额:$ 7.1万
- 依托单位:
- 依托单位国家:日本
- 项目类别:Grant-in-Aid for Scientific Research on Priority Areas
- 财政年份:2004
- 资助国家:日本
- 起止时间:2004 至 2007
- 项目状态:已结题
- 来源:
- 关键词:
项目摘要
In this project, taking microporous coordination polymers as an example, we estimate and clarify the microscopic properties of the pores in materials on the basis of molecular orbital (M0) theory and density functional theory (DFT). Further, through molecular mechanical (MM) and monte carlo (MC) simulation, we will survey the guideline to design the coordination space by investigating the correspondence between the macroscopic and the microscopic ones.[Results] 1) Microscopic properties of microporous coordination polymer CPL-1 On the basis of Universal Force Field (UFF), we recalibrated the force-field parameters of 02 for the purpose to describe the thermodynamic behaviors satisfactorily, e.g., the ladder structure of 02 dimers in nanochannels in CPL-1. Then, the effective potential of 02-02 interaction was expressed as V02-02, a summation of van der Waals VvdW and quadrupole interaction VEQQ. By fitting V02-02 to the ab initio data, a set of parameters D0-0, Re0-0 and q0 for an oxyg … More en atom of 02 molecule were obtained, i. e., 59.4762 K, 5.9943 a0 and -0.2227 e, respectively.In addition, q0 could be obtained directly as -0.2518 e at the MP2/6-31G+(d) level of theory by utilizing Gaussian03, so that it could reproduce reasonably the quadrupole moment of 02 and, then, corresponds to the fitting q0 value.2) Reaction mechanism in specific polymerization in CPL-2 It can be understood that the molecular mechanically optimized structure by using the UFF should also reproduce a specific hydrogen-bonding interaction between an methyl propiolate (MP) monomer and two oxygen atoms in the carboxylate moiety in CPL-2. The -C ≡ CH group of MP is clearly oriented towards the carboxylate oxygen atoms on the pore wall, and the acetylenic hydrogen atom and the oxygen atoms are close enough for an efficient hydrogen bonding (2.8 and 2.9 Å), which is consistent with the experimental results. A schematic illustration is shown in Ref.3 for randomly-aligned MP molecules in the nanochannel in CPL-2, which are found closely-packed in fact for controlling the stereostructure(the cis and trans chain sequence).[References](l) Y. Ohta, H. Hitomi, M. Nagaoka, R. Matsuda and S. Kitagawa, J. Amer. Chem. Soc. 2007, submitted.(2) (a) T. Uemura, R. Kitaura, Y. Ohta, M. Nagaoka, S. Kitagawa, Angew. Chem. 2006, 118, 4218; (b) Angew. Chem. Int. Ed. 2006, 45, 4112.(3) M. Nagaoka, Y. Ohta and H. Hitomi, Coord. Chem. Rev., 2007, 251, 2522. Less
本课题以微孔配位聚合物为例,基于分子轨道理论和密度泛函理论,对材料中孔隙的微观性质进行了估算和澄清。[结果]1)微孔配位聚合物CPL-1的微观性质在万有力场(UFF)的基础上,我们重新标定了02的力场参数,以便较好地描述CPL-1中02二聚体在纳米通道中的梯形结构等热力学行为。然后,02-02相互作用的有效势被表示为V02-02,它是范德华相互作用VvdW和四极相互作用VEQQ的总和。通过将V02-02拟合到从头算数据,用于OGG…的一组参数D0-0、RE0-0和Q0得到了较多的02分子的En原子,分别为59.4762 K,5.9943 a0和-0.2227 e。另外,利用Gaussian03可以在MP2/6-31G+(D)的理论水平上直接得到-0.2518 e,从而合理地再现了02分子的四极矩。2)CPL-2中特定聚合的反应机理可以理解,使用UFF的分子力学优化结构也应该重现CPL-2中丙酸甲酯(MP)单体和羧酸盐部分中的两个氧原子之间的特定氢键相互作用。MP分子中的-C≡CH基团明显朝向孔壁上的羧基氧原子,乙酰氢原子和氧原子距离足够近,可以形成有效的氢键(2.8和2.9Å),这与实验结果是一致的.参考文献3给出了CPL-2中纳米通道中随机排列的MP分子的示意图,这些分子实际上是紧密堆积的,用于控制立体结构(顺式和反式链序列)。化学。SoC。(2)(A)T.Uemura,R.Kitaura,Y.Ohta,M.Nagaoka,S.Kitagawa,Angew.化学。2006年,118,4218;(B)Angew。化学。内部艾德2006年,45,4112。(3)M.Nagaoka,Y.Ohta和H.Hitomi,Coord。化学。Rev.,2007,251,2522.较少
项目成果
期刊论文数量(59)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
表面Kirkwood-Buff法による補償溶質エクトイン選択的排除の分子論的理解
表面 Kirkwood-Buff 法选择性排除补偿性溶质四氢嘧啶的分子理解
- DOI:
- 发表时间:2008
- 期刊:
- 影响因子:0
- 作者:優乙石;長岡正隆
- 通讯作者:長岡正隆
Structural Optimization of Ammonia Ionization Process in Aqueous Solution via Free Energy Gradient Method
自由能梯度法优化水溶液中氨电离过程的结构
- DOI:
- 发表时间:2007
- 期刊:
- 影响因子:0
- 作者:Y. Koyano;N. Takenaka;Y. Nakagawa;M. Nagaoka
- 通讯作者:M. Nagaoka
Coarse-Grained Approach to Nonequilibrium Molecular Dynamics : Application to Relaxation process of Vibrationally Excited Hydrogen Fluoride in aqueous Solution
非平衡分子动力学的粗粒度方法:应用于水溶液中振动激发氟化氢的弛豫过程
- DOI:
- 发表时间:2005
- 期刊:
- 影响因子:0
- 作者:T.Okamoto;M.Nagaoka
- 通讯作者:M.Nagaoka
Transition-State Characterization of Ammonia Ionization Process in Aqueous Solution via Free-Energy Gradient Method
自由能梯度法表征水溶液中氨电离过程的过渡态
- DOI:
- 发表时间:2006
- 期刊:
- 影响因子:0
- 作者:早坂 良;秋山 裕俊;杉森 隼人;北山 真太郎;鈴木 正人;落水浩一郎;M.Motosuke;早坂 良;元祐 昌廣;M.Motosuke;M.Motosuke;M.Motosuke;元祐 昌廣;早坂 良;早坂 良;早坂 良;早坂 良;長岡 正隆
- 通讯作者:長岡 正隆
Nanochannel-promoted polymerization of substituted acetylenes in porous coordination polymers.
- DOI:10.1002/anie.200600333
- 发表时间:2006-06
- 期刊:
- 影响因子:0
- 作者:T. Uemura;R. Kitaura;Y. Ohta;M. Nagaoka;S. Kitagawa
- 通讯作者:T. Uemura;R. Kitaura;Y. Ohta;M. Nagaoka;S. Kitagawa
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NAGAOKA Masataka其他文献
Performance Research of Clustering Methods for Detecting State Transition Trajectories in Hemoglobin
检测血红蛋白状态转换轨迹的聚类方法的性能研究
- DOI:
10.2477/jccj.2021-0014 - 发表时间:
2020 - 期刊:
- 影响因子:0
- 作者:
TAKAMI Kei;KITAMURA Yukichi;NAGAOKA Masataka - 通讯作者:
NAGAOKA Masataka
Data Scientific Study on Allosteric Regulation of Hemoglobin -The Role of Chloride Ion in Quaternary Structural Change-
血红蛋白变构调节的数据科学研究-氯离子在第四纪结构变化中的作用-
- DOI:
10.2477/jccj.2021-0045 - 发表时间:
2021 - 期刊:
- 影响因子:0
- 作者:
TANAKA Miho;TAKAHASHI Yume;TAKAMI Kei;KITAMURA Yukichi;NAGAOKA Masataka - 通讯作者:
NAGAOKA Masataka
NAGAOKA Masataka的其他文献
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{{ truncateString('NAGAOKA Masataka', 18)}}的其他基金
Challenge to porous polymeric membrane synthesis by micro simulation
微模拟对多孔聚合物膜合成的挑战
- 批准号:
24654137 - 财政年份:2012
- 资助金额:
$ 7.1万 - 项目类别:
Grant-in-Aid for Challenging Exploratory Research
New Development of Kramers-Fokker-Planck Equation of Polyatomic Molecules
多原子分子Kramers-Fokker-Planck方程的新进展
- 批准号:
20550011 - 财政年份:2008
- 资助金额:
$ 7.1万 - 项目类别:
Grant-in-Aid for Scientific Research (C)
New Development of Reaction Dynamics Theory based on the Free Energy Gradient Method
基于自由能梯度法的反应动力学理论新进展
- 批准号:
15350010 - 财政年份:2003
- 资助金额:
$ 7.1万 - 项目类别:
Grant-in-Aid for Scientific Research (B)
MOLECULAR DYNAMICS STUDY ON REAGENT DENSITY DEPENDENCE AND TEMPERATURE-PRESSURE EFFECT IN SOLUTION CHEMICAL REACTIONS
溶液化学反应中试剂密度依赖性和温压效应的分子动力学研究
- 批准号:
13440176 - 财政年份:2001
- 资助金额:
$ 7.1万 - 项目类别:
Grant-in-Aid for Scientific Research (B)
THEORICAL STUDY ON FUNDAMENTAL THEORIES ON MULTI-DIMENSIONAL CHEMICALLY REACTING SYSTEMS
多维化学反应系统基础理论的理论研究
- 批准号:
11440174 - 财政年份:1999
- 资助金额:
$ 7.1万 - 项目类别:
Grant-in-Aid for Scientific Research (B).
THEORICAL STUDY ON FUNDAMENTAL THEORIES ON MULTI-DIMENSIONAL CHEMICALLY REACTING SYSTEMS
多维化学反应系统基础理论的理论研究
- 批准号:
10044106 - 财政年份:1998
- 资助金额:
$ 7.1万 - 项目类别:
Grant-in-Aid for Scientific Research (B).