Temperature and pH driven association in uranyl aqueous solutions

被引:6
作者
Druchok, M. [1 ]
Holovko, M. [1 ]
机构
[1] NAS Ukraine, Inst Condensed Matter Phys, UA-79011 Lvov, Ukraine
关键词
molecular dynamics; uranyl aqueous solution; association; pH; temperature; MOLECULAR-DYNAMICS; HYDRATION; CATION; 18-CROWN-6; ADDUCTS; UO22+; WATER; MODEL;
D O I
10.5488/CMP.15.43602
中图分类号
O469 [凝聚态物理学];
学科分类号
070205 ;
摘要
An association behavior of uranyl ions in aqueous solutions is explored. For this purpose a set of all-atom molecular dynamics simulations is performed. During the simulation, the fractions of uranyl ions involved in dimer and trimer formations were monitored. To accompany the fraction statistics one also collected distributions characterizing average times of the dimer and trimer associates. Two factors effecting the uranyl association were considered: temperature and pH. As one can expect, an increase of the temperature decreases an uranyl capability of forming the associates, thus lowering bound fractions/times and vice versa. The effect of pH was modeled by adding H+ or OH- ions to a "neutral" solution. The addition of hydroxide ions OH- favors the formation of the associates, thus increasing bound times and fractions. The extra H+ ions in a solution produce an opposite effect, thus lowering the uranyl association capability. We also made a structural analysis for all the observed associates to reveal the mutual orientation of the uranyl ions.
引用
收藏
页数:9
相关论文
共 21 条
[1]  
Ahearne J.F., 1997, PHYS TODAY, V50, P27, DOI [10.1063/1.881763, DOI 10.1063/1.881763]
[2]   A molecular dynamics study of uranyl hydration [J].
Druchok, M ;
Bryk, T ;
Holovko, M .
JOURNAL OF MOLECULAR LIQUIDS, 2005, 120 (1-3) :11-14
[3]  
Druchok M. Yu., 2003, Journal of Physical Studies, V7, P402
[4]   STRUCTURE AND PROPERTIES OF THE CF1 CENTRAL FORCE MODEL OF WATER - INTEGRAL-EQUATION THEORY [J].
DUH, DM ;
PERERA, DN ;
HAYMET, ADJ .
JOURNAL OF CHEMICAL PHYSICS, 1995, 102 (09) :3736-3746
[5]   Molecular dynamics study of aqueous uranyl interactions with quartz (010) [J].
Greathouse, JA ;
O'Brien, RJ ;
Bemis, G ;
Pabalan, RT .
JOURNAL OF PHYSICAL CHEMISTRY B, 2002, 106 (07) :1646-1655
[6]   HYDRATION OF UO2(2+) CATION AND ITS NO3(-) AND 18-CROWN-6 ADDUCTS STUDIED BY MOLECULAR-DYNAMICS SIMULATIONS [J].
GUILBAUD, P ;
WIPFF, G .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (21) :5685-5692
[7]   Force field representation of the UO22+ cation from free energy MD simulations in water. Tests on its 18-crown-6 and NO3- adducts, and on its calix[6]arene(6-) and CMPO complexes [J].
Guilbaud, P ;
Wipff, G .
JOURNAL OF MOLECULAR STRUCTURE-THEOCHEM, 1996, 366 (1-2) :55-63
[8]  
HAYLE JM, 1992, MOL DYNAMICS SIMULAT
[9]   A molecular dynamics study of the hydrated-hydrolyzed structure of multivalent cations based on the model of primitive cation [J].
Holovko, M. ;
Druchok, M. ;
Bryk, T. .
JOURNAL OF MOLECULAR LIQUIDS, 2007, 131 :65-71
[10]   Primitive model for cation hydrolysis: A molecular-dynamics study [J].
Holovko, M ;
Druchok, M ;
Bryk, T .
JOURNAL OF CHEMICAL PHYSICS, 2005, 123 (15)