Microscopic Investigation of Ethylene Carbonate Interface: A Molecular Dynamics and Vibrational Spectroscopic Study

Citation: WANG Lin, XIN Liang, ISHIYAMA Tatsuya, PENG Qiling, YE Shen, MORITA Akihiro. Microscopic Investigation of Ethylene Carbonate Interface: A Molecular Dynamics and Vibrational Spectroscopic Study[J]. Acta Physico-Chimica Sinica, 2018, 34(10): 1124-1135. doi: 10.3866/PKU.WHXB201801291 shu

Microscopic Investigation of Ethylene Carbonate Interface: A Molecular Dynamics and Vibrational Spectroscopic Study

1.
Department of Chemistry, Graduate School of Science, Tohoku University, Aoba-ku, Sendai 980-8578, Japan
2.
Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, Kyoto 615-8520, Japan
3.
Department of Applied Chemistry, Graduate School of Science and Engineering, University of Toyama, Toyama 930-8555, Japan
4.
Institute for Catalysis, Hokkaido University, Kita-ku, Sapporo 001-0021, Japan

通讯作者: MORITAAkihiro, morita@tohoku.ac.jp

摘要: Ethylene carbonate (EC) liquid and its vapor-liquid interface were investigated using a combination of molecular dynamics (MD) simulation and vibrational IR, Raman and sum frequency generation (SFG) spectroscopies. The MD simulation was performed with a flexible and polarizable model of the EC molecule newly developed for the computation of vibrational spectra. The internal vibration of the model was described on the basis of the harmonic couplings of vibrational modes, including the anharmonicity and Fermi resonance coupling of C＝O stretching. The polarizable model was represented by the charge response kernel (CRK), which is based on ab initio molecular orbital calculations and can be readily applied to other systems. The flexible and polarizable model can also accurately reproduce the structural and thermodynamic properties of EC liquid. Meanwhile, a comprehensive set of vibrational spectra of EC liquid, including the IR and Raman spectra of the bulk liquid as well as the SFG spectra of the liquid interface, were experimentally measured and reported. The set of experimental vibrational spectra provided valuable information for validating the model, and the MD simulation using the model comprehensively elucidates the observed vibrational IR, Raman, and SFG spectra of EC liquid. Further MD analysis of the interface region revealed that EC molecules tend to orientate themselves with the C＝O bond parallel to the interface. The MD simulation explains the positive Im[$ \chi ^{(2)}$](ssp) band of the C＝O stretching region in the SFG spectrum in terms of the preferential orientation of EC molecules at the interface. This work also elucidates the distinct lineshapes of the C＝O stretching band in the IR, Raman, and SFG spectra. The lineshapes of the C＝O band are split by the Fermi resonance of the C＝O fundamental and the overtone of skeletal stretching. The Fermi resonance of C＝O stretching was fully analyzed using the empirical potential parameter shift analysis (EPSA) method. The apparently different lineshapes of the C＝O stretching band in the IR, Raman, and SFG spectra were attributed to the frequency shift of the C＝O fundamental in different solvation environments in the bulk liquid and at the interface. This work proposes a systematic procedure for investigating the interface structure and SFG spectra, including general modeling procedure based on ab initio calculations, validation of the model using available experimental data, and simultaneous analysis of molecular orientation and SFG spectra through MD trajectories. The proposed procedure provides microscopic information on the EC interface in this study, and can be further applied to investigate other interface systems, such as liquid-liquid and solid-liquid interfaces.

关键词:

Ethylene carbonate
/ SFG
/ Fermi resonance
/ EPSA

English

Microscopic Investigation of Ethylene Carbonate Interface: A Molecular Dynamics and Vibrational Spectroscopic Study

1.
Department of Chemistry, Graduate School of Science, Tohoku University, Aoba-ku, Sendai 980-8578, Japan
2.
Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, Kyoto 615-8520, Japan
3.
Department of Applied Chemistry, Graduate School of Science and Engineering, University of Toyama, Toyama 930-8555, Japan
4.
Institute for Catalysis, Hokkaido University, Kita-ku, Sapporo 001-0021, Japan

Corresponding author: MORITA Akihiro, morita@tohoku.ac.jp

Received Date: 26 December 2017
Accepted Date: 22 January 2018
Revised Date: 22 January 2018
Available Online: 15 October 2018
Fund Project:
This work was supported by Elements Strategy Initiative for Catalysts and Batteries, Kyoto University, Cooperative Research Program of Institute for Catalysis, Hokkaido University, Japan and the Grants-in-Aids (JP25104003, JP26288003) by the Japan Society for the Promotion of Science (JSPS) and Ministry of Education, Culture, Sports and Technology (MEXT), Japan

Abstract: Ethylene carbonate (EC) liquid and its vapor-liquid interface were investigated using a combination of molecular dynamics (MD) simulation and vibrational IR, Raman and sum frequency generation (SFG) spectroscopies. The MD simulation was performed with a flexible and polarizable model of the EC molecule newly developed for the computation of vibrational spectra. The internal vibration of the model was described on the basis of the harmonic couplings of vibrational modes, including the anharmonicity and Fermi resonance coupling of C＝O stretching. The polarizable model was represented by the charge response kernel (CRK), which is based on ab initio molecular orbital calculations and can be readily applied to other systems. The flexible and polarizable model can also accurately reproduce the structural and thermodynamic properties of EC liquid. Meanwhile, a comprehensive set of vibrational spectra of EC liquid, including the IR and Raman spectra of the bulk liquid as well as the SFG spectra of the liquid interface, were experimentally measured and reported. The set of experimental vibrational spectra provided valuable information for validating the model, and the MD simulation using the model comprehensively elucidates the observed vibrational IR, Raman, and SFG spectra of EC liquid. Further MD analysis of the interface region revealed that EC molecules tend to orientate themselves with the C＝O bond parallel to the interface. The MD simulation explains the positive Im[$ \chi ^{(2)}$](ssp) band of the C＝O stretching region in the SFG spectrum in terms of the preferential orientation of EC molecules at the interface. This work also elucidates the distinct lineshapes of the C＝O stretching band in the IR, Raman, and SFG spectra. The lineshapes of the C＝O band are split by the Fermi resonance of the C＝O fundamental and the overtone of skeletal stretching. The Fermi resonance of C＝O stretching was fully analyzed using the empirical potential parameter shift analysis (EPSA) method. The apparently different lineshapes of the C＝O stretching band in the IR, Raman, and SFG spectra were attributed to the frequency shift of the C＝O fundamental in different solvation environments in the bulk liquid and at the interface. This work proposes a systematic procedure for investigating the interface structure and SFG spectra, including general modeling procedure based on ab initio calculations, validation of the model using available experimental data, and simultaneous analysis of molecular orientation and SFG spectra through MD trajectories. The proposed procedure provides microscopic information on the EC interface in this study, and can be further applied to investigate other interface systems, such as liquid-liquid and solid-liquid interfaces.

Key words:

Ethylene carbonate
/ SFG
/ Fermi resonance
/ EPSA

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

Microscopic Investigation of Ethylene Carbonate Interface: A Molecular Dynamics and Vibrational Spectroscopic Study

通讯作者: MORITAAkihiro, morita@tohoku.ac.jp

English

Microscopic Investigation of Ethylene Carbonate Interface: A Molecular Dynamics and Vibrational Spectroscopic Study

Corresponding author: MORITA Akihiro, morita@tohoku.ac.jp

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Microscopic Investigation of Ethylene Carbonate Interface: A Molecular Dynamics and Vibrational Spectroscopic Study

通讯作者: MORITAAkihiro, morita@tohoku.ac.jp

English

Microscopic Investigation of Ethylene Carbonate Interface: A Molecular Dynamics and Vibrational Spectroscopic Study

Corresponding author: MORITA Akihiro, morita@tohoku.ac.jp

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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