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题名: Determination of structure and energetics for Gibbs surface adsorption layers of binary liquid mixture 2. Methanol plus water
作者: Chen, H;  Gan, W;  Lu, R;  Guo, Y;  Wang, HF
刊名: JOURNAL OF PHYSICAL CHEMISTRY B
发表日期: 2005-04-28
DOI: 10.1021/jp0501906
卷: 109, 期:16, 页:8064-8075
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: Vapor/methanol and vapor/methanol-water mixture interfaces have been among the benchmark liquid interfaces under extensive experimental and theoretical investigation. In this report, we studied the orientation, structure and energetics of the vapor/methanol-water interface with newly developed techniques in sum frequency generation vibrational spectroscopy (SFG-VS). Different from the interpretations in previous SFG-VS studies for a more disordered interface at higher bulk methanol concentrations, we found that the methanol-water mixture interface is well ordered in the whole concentration region. We are able to do so because direct polarization null angle (PNA) measurement allowed us to accurately determine the CH3 orientation at the interface and to separate the orientational and interface density contributions to the SFG-VS signal. We found that the CH3 groups at the interface pointed out almost perpendicularly from the interface. We further found that this well-ordered vapor/methanol-water mixture interface has an antiparallel structure. With the double layer adsorption model (DAM) and Langmuir isotherm, the adsorption free energies for the first and second layer are obtained as -1.7 +/- 0.1 kcal/mol and 0.5 +/- 0.4 kcal/mol, respectively. Therefore, the second layer adsorption is slightly negative, and this means that replacement of the second layer water molecule with methanol molecule is energetically unfavorable. Comparing this interface with the vapor/acetone-water mixture interface reported previously, we are able to correlate the second layer adsorption free energy with the work of self-association using the pairwise self- and mutual interaction energies between the water and solute molecules. These results provided detailed microscopic structural evidences for understanding of liquid interfaces.
关键词[WOS]: SUM-FREQUENCY GENERATION ;  MONTE-CARLO SIMULATION ;  CH STRETCHING MODES ;  VAPOR INTERFACE ;  VIBRATIONAL SPECTROSCOPY ;  MOLECULAR-DYNAMICS ;  2ND-HARMONIC GENERATION ;  ORIENTATIONAL ORDER ;  ACETONE ;  CLUSTERS
语种: 英语
WOS记录号: WOS:000228603700066
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/139692
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Inst Chem, State Key Lab Mol React Dynam, Beijing 100080, Peoples R China

Recommended Citation:
Chen, H,Gan, W,Lu, R,et al. Determination of structure and energetics for Gibbs surface adsorption layers of binary liquid mixture 2. Methanol plus water[J]. JOURNAL OF PHYSICAL CHEMISTRY B,2005,109(16):8064-8075.
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