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题名: Characterization of protonated formamide-containing clusters by infrared spectroscopy and ab initio calculations. II. Hydration of formamide in the gas phase
作者: Chaudhuri, C;  Jiang, JC;  Wu, CC;  Wang, X;  Chang, HC
刊名: JOURNAL OF PHYSICAL CHEMISTRY A
发表日期: 2001-10-04
DOI: 10.1021/jp004103f
卷: 105, 期:39, 页:8906-8915
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical ;  Physics, Atomic, Molecular & Chemical
研究领域[WOS]: Chemistry ;  Physics
英文摘要: Structures of the solvation shells of O-protonated formamide (H(+)FA) have been characterized by infrared spectroscopy and ab initio calculations at varying stages of hydration. A few isomeric structures, including both H(+)FA- and H3O+-centered forms, were identified from a close examination of the hydrogen-bonded and non-hydrogen-bonded NH and OH stretching spectra of H(+)FA(H2O)(n) (n = 3 and 4) produced by a supersonic expansion. Theoretical investigations of H(+)FA(H2O)(1-3) indicate that filling of the first hydration shell of the protonated formamide cation with three water molecules is not an energetically favorable process. The process is hampered by the hydrogen bond anticooperative effect, which prohibits both NH bonds to be involved in hydrogen bonding. Further increasing the cluster size to n = 4 results in grouping of the water molecules on one side of the formamide, rather than forming a filled first solvation shell of H(+)FA. The grouping, in effect, enhances the proton affinity of the water molecule in direct contact with the excess proton and progressively moves th proton away from H(+)FA, producing an H3O+ ion core. Detailed analysis of the results, both qualitatively and quantitatively, reveals the existence of a low-barrier proton transfer process, which is expected to occur similarly in aqueous solutions 'during acid-catalyzed amide hydrolysis. In this work, we also successfully identified a shell-filled isomer for H+(FA)(3)H2O for the first time. It is demonstrated that a combined investigation of cluster ions by infrared spectroscopy and ab initio calculations allows for an unambiguous determination of both the protonation sites and hydration structures of biomolecules in the gas phase.
关键词[WOS]: EXCESS PROTON ;  AMIDE HYDROLYSIS ;  WATER CLUSTERS ;  O-PROTONATION ;  HYDROGEN-BOND ;  IONS ;  ACID ;  COMPLEXES ;  EXCHANGE ;  ELECTROSPRAY
语种: 英语
WOS记录号: WOS:000171401200010
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/138847
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.Acad Sinica, Inst Atom & Mol Sci, Taipei 106, Taiwan
2.Natl Taiwan Univ, Dept Chem, Taipei 106, Taiwan
3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China

Recommended Citation:
Chaudhuri, C,Jiang, JC,Wu, CC,et al. Characterization of protonated formamide-containing clusters by infrared spectroscopy and ab initio calculations. II. Hydration of formamide in the gas phase[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2001,105(39):8906-8915.
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