Coordination variation of hydrated Cu2+/Br1- ions traversing the interfacial water in mesopores | |
Wang, Q ; Huang, XF ; Li, CX ; Pan, LQ ; Wu, ZH ; Hu, TD ; Jiang, Z ; Huang, YY ; Cao, ZX ; Sun, G ; Lu, KQ | |
刊名 | AIP ADVANCES |
2012 | |
卷号 | 2期号:2 |
关键词 | RAY-ABSORPTION SPECTROSCOPY AQUEOUS-SOLUTIONS MOLECULAR-DYNAMICS ZSM-5 ZEOLITES FINE-STRUCTURE AQUA ION COPPER ADSORPTION SURFACES BROMIDE |
ISSN号 | 2158-3226 |
通讯作者 | Cao, ZX: Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China. |
中文摘要 | Resolution of the atomistic and electronic details about the coordination structure variation of hydrated ions in the interfacial water is still a tough challenge, which is, however, essentially important for the understanding of ion adsorption, permeation and other similar processes in aqueous solutions. Here we report the tracing of coordination structure variation for hydrated Cu2+/Br1- ions traversing the interfacial water in Vycor mesopores (phi = 7.6 nm) by employing both X-ray absorption near edge structure and extended X-ray absorption fine structure spectroscopies. By controlled desorption/adsorption of water, the filling fraction of the mesopores, thus the water layer thickness, can be adjusted, which in turn effects the variation of coordination structure of the ions therein. It is found that both Cu2+ and Br1- ions prefer staying exclusively in the core water, and in this circumstance no ion pairs have been detected in the solution of concentrations up to 1.0 M. Following capillary decondensation occurring at a filling fraction of similar to 35% which corresponds to a water layer of about three monolayers, Br1- ions begin immediately to reconstruct their first coordination shell, characterized by ionic dehydration, shrinkage of ion-water bond length, and formation of ion pairs. In contrast, Cu2+ ions can retain a bulk-like coordination structure till being driven to bond directly to the pore surface when the filling fraction is below 20%. At the final stage of dehydration via thermal vacuum treatment at 110 degrees C, Cu2+ ions can be completely reduced to the Cu1+ state, and recover at room temperature only when the filling fraction is above 14%. These results may be inspirable for the investigation of similar problems concerning hydrated ions in water solution under different confining conditions. Copyright 2012 Author(s). This article is distributed under a Creative Commons Attribution 3.0 Unported License. [http://dx.doi.org/10.1063/1.4704545] |
收录类别 | SCI |
资助信息 | NSFC [10874208, 50971023]; National Basic Research Program of China [2010CB630705, 2009CB930801]; Knowledge Innovation Project of Chinese Academy of Sciences on Water Science Research |
语种 | 英语 |
公开日期 | 2013-09-17 |
内容类型 | 期刊论文 |
源URL | [http://ir.iphy.ac.cn/handle/311004/35185] |
专题 | 物理研究所_物理所公开发表论文_物理所公开发表论文_期刊论文 |
推荐引用方式 GB/T 7714 | Wang, Q,Huang, XF,Li, CX,et al. Coordination variation of hydrated Cu2+/Br1- ions traversing the interfacial water in mesopores[J]. AIP ADVANCES,2012,2(2). |
APA | Wang, Q.,Huang, XF.,Li, CX.,Pan, LQ.,Wu, ZH.,...&Lu, KQ.(2012).Coordination variation of hydrated Cu2+/Br1- ions traversing the interfacial water in mesopores.AIP ADVANCES,2(2). |
MLA | Wang, Q,et al."Coordination variation of hydrated Cu2+/Br1- ions traversing the interfacial water in mesopores".AIP ADVANCES 2.2(2012). |
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