Institutional Repository of Anhui Institute of Optics and Fine Mechanics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei, Anhui 230031, China
| Examining the structural evolution of bicarbonate-water clusters: insights from photoelectron spectroscopy, basin-hopping structural search, and comparison with available IR spectral studies | |
Wen, Hui1,2; Hou, Gao-Lei2; Liu, Yi-Rong1 ; Wang, Xue-Bin2; Huang, Wei1,3
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| 2016-07-14 | |
| 发表期刊 | PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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| 摘要 | Bicarbonate plays a crucial biochemical role in the physiological pH buffering system and also has important atmospheric implications. In the current study, HCO3- (H2O)(n) (n = 0-13) clusters were successfully produced via electrospray ionization of the corresponding bulk salt solution, and were characterized by negative ion photoelectron spectroscopy and theoretical calculations. Photoelectron spectra reveal that the electron binding energy monotonically increases with the cluster size up to n = 10 and remains largely the same after n 4 > 10. The photo-detaching feature of the solute HCO3- itself, which dominates in the small clusters, diminishes with the increase of water coverage. Based on the charge distribution and molecular orbital analyses, the universal high electron binding energy tail that dominates in the larger clusters can be attributed to the ionization of water. Thus, the transition of ionization from the solute to the solvent at a size larger than n = 10 has been observed. Extensive theoretical structural search based on the basin-hopping unbiased method was carried out, and a plethora of low energy isomers have been obtained for each medium and large-sized cluster. By comparing the simulated photoelectron spectra and calculated electron binding energies with the experiments, as well as by comparing the simulated infrared spectra with previously reported IR spectra, the best fit structures and the structural evolutionary routes are presented. The nature of bicarbonate-water interactions is mainly electrostatic as implied by electron localization function (ELF) analysis. |
| 文章类型 | Article |
| WOS标题词 | Science & Technology ; Physical Sciences |
| DOI | 10.1039/c6cp01542e |
| 关键词[WOS] | GENERALIZED GRADIENT APPROXIMATION ; MOLECULAR-DYNAMICS SIMULATIONS ; DOUBLY-CHARGED ANION ; SODIUM-BICARBONATE ; GAS-PHASE ; INFRARED PHOTODISSOCIATION ; THERMOCHEMICAL PROPERTIES ; CATALYTIC MECHANISM ; EXCITATION-ENERGIES ; CARBONIC-ANHYDRASE |
| 收录类别 | SCI |
| 语种 | 英语 |
| 项目资助者 | U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; Division of Chemical Sciences, Geosciences, and Biosciences ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; DOE's Office of Biological and Environmental Research ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; National Natural Science Foundation of China(21403244 ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; State Key Program of National Natural Science of China(21133008) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; National High Technology Research and Development Program of China (863 Program)(2014AA06A501) ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; "Interdisciplinary and Cooperative Team" of CAS ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 21573241 ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) ; 41527808) |
| WOS研究方向 | Chemistry ; Physics |
| WOS类目 | Chemistry, Physical ; Physics, Atomic, Molecular & Chemical |
| WOS记录号 | WOS:000379482100042 |
| 引用统计 | |
| 文献类型 | 期刊论文 |
| 条目标识符 | http://ir.hfcas.ac.cn:8080/handle/334002/21514 |
| 专题 | 中科院安徽光学精密机械研究所 |
| 作者单位 | 1.Chinese Acad Sci, Anhui Inst Opt & Fine Mech, Lab Atmospher Physicochem, Hefei 230031, Anhui, Peoples R China 2.Pacific NW Natl Lab, Div Phys Sci, POB 999,MS K8-88, Richland, WA 99352 USA 3.Univ Sci & Technol China, Sch Environm Sci & Optoelect Technol, Hefei 230026, Anhui, Peoples R China |
| 第一作者单位 | 中科院安徽光学精密机械研究所 |
| 推荐引用方式 GB/T 7714 | Wen, Hui,Hou, Gao-Lei,Liu, Yi-Rong,et al. Examining the structural evolution of bicarbonate-water clusters: insights from photoelectron spectroscopy, basin-hopping structural search, and comparison with available IR spectral studies[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2016,18(26):17470-17482. |
| APA | Wen, Hui,Hou, Gao-Lei,Liu, Yi-Rong,Wang, Xue-Bin,&Huang, Wei.(2016).Examining the structural evolution of bicarbonate-water clusters: insights from photoelectron spectroscopy, basin-hopping structural search, and comparison with available IR spectral studies.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,18(26),17470-17482. |
| MLA | Wen, Hui,et al."Examining the structural evolution of bicarbonate-water clusters: insights from photoelectron spectroscopy, basin-hopping structural search, and comparison with available IR spectral studies".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 18.26(2016):17470-17482. |
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