期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 13, 期 29, 页码 13305-13309出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c0cp03005h
关键词
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资金
- National Science Foundation of China [41002013, 40973029]
- National Priority Development Project Fundamental Research [2007CB815603]
- State Key Laboratory for Mineral Deposits Research, Nanjing University [2008-II-14, 2009-II-3]
With ab initio molecular dynamics simulations, the free-energy profiles of hydrated Zn2+ are calculated for both gaseous and aqueous systems from ambient to supercritical conditions, and from the derived free-energy information, the speciation of hydrated Zn2+ has been revealed. It is shown that the 4, 5 and 6 fold complexes coexist in both phases at ambient condition. As T-P increases a clear trend is found for both phases: the 6 fold states gradually become unstable and cannot exist stably any more over 620 K, but in contrast, the 4 and 5 fold states can hold up to 1000 K with similar probabilities. It is found that the stability of the 4 and 5 fold states has an entropic origin. This study constitutes a relatively complete speciation picture for aqua-zinc complexes over a broad T-P range.
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