铯在叶蜡石孔隙中吸附与扩散的分子动力学研究
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摘要
本文采用分子动力学方法(molecular dynamics, MD)模拟研究了Cs~+在叶蜡石纳米孔隙中的吸附和扩散行为.径向分布函数和配位数的分析表明,在叶蜡石孔隙中Cs~+的第一水合壳层半径为3.05?,水合数为8.0～8.5.原子密度分布表明Cs~+是以外层表面络合物的形式吸附在叶蜡石基面上. Cs~+的水合结构及其吸附百分比受浓度和温度的影响均较小.随着温度升高, Cs~+热运动加剧导致其扩散系数显著增大.
In the article, molecular dynamics simulations are carried out to investigate the adsorption and diffusion behaviors of Cs~+in pyrophyllite nanopore. The results of radial distribution function and coordination number indicate that the first hydration shell radius of Cs~+and hydration number are 3.05 ? and 8.0～8.5, respectively. Atomic density profiles demonstrate that Cs~+adsorbed on the pyrophyllite basal in the form of outer-sphere surface complex. And the concentration and temperature have little impact on the hydrated structure and adsorption percent of Cs~+. Increasing temperature will promote the thermal motion of Cs~+, which leads to diffusion coefficient increased dramatically.
In the article, molecular dynamics simulations are carried out to investigate the adsorption and diffusion behaviors of Cs~+in pyrophyllite nanopore. The results of radial distribution function and coordination number indicate that the first hydration shell radius of Cs~+and hydration number are 3.05 ? and 8.0～8.5, respectively. Atomic density profiles demonstrate that Cs~+adsorbed on the pyrophyllite basal in the form of outer-sphere surface complex. And the concentration and temperature have little impact on the hydrated structure and adsorption percent of Cs~+. Increasing temperature will promote the thermal motion of Cs~+, which leads to diffusion coefficient increased dramatically.
引文
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2 Omar H,Arida H,Daifullah A.Appl Clay Sci,2009,44:21-26
3 Yang S,Okada N,Nagatsu M.J Hazard Mater,2016,301:8-16
4 Cygan RT,Liang JJ,Kalinichev AG.J Phys Chem B,2004,108:1255-1266
5 Sun L,Tanskanen JT,Hirvi JT,Kasa S,Schatz T,Pakkanen TA.Chem Phys,2015,455:23-31
6 Zhang S,Liu Q,Gao F,Li X,Liu C,Li H,Boyd SA,Johnston CT,Teppen BJ.J Phys Chem C,2017,121:402-409
7 Zhao Q,Burns SE.Colloids Surfs A,2017,516:354-361
8 Zhang TN,Xu XW,Dong L,Tan ZY,Liu CL.Acta Phys-Chim Sin,2017,33:2013-2021(in Chinese)[张陶娜,徐雪雯,董亮,谭昭怡,刘春立.物理化学学报,2017,33:2013-2021]
9 Kerisit S,Okumura M,Rosso KM,Machida M.Clay Clay Miner,2016,64:389-400
10 Kosakowski G,Churakov SV,Thoenen T.Clay Clay Miner,2008,56:190-206
11 Churakov SV.Environ Sci Technol,2013,47:9816-9823
12 Lammers LN,Bourg IC,Okumura M,Kolluri K,Sposito G,Machida M.J Colloid Interface Sci,2017,490:608-620
13 Kadoura A,Narayanan Nair AK,Sun S.J Phys Chem C,2016,120:12517-12529
14 Pérez-Conesa S,Martínez JM,Sánchez Marcos E.J Phys Chem C,2017,121:27437-27444
15 Lee JH,Guggenheim S.Am Mineral,1981,66:350-357
16 Plimpton S.J Comput Phys,1995,117:1-19
17 Berendsen HJC,Grigera JR,Straatsma TP.J Phys Chem,1987,91:6269-6271
18 Ryckaert JP,Ciccotti G,Berendsen HJC.J Comput Phys,1977,23:327-341
19 Dang LX.Chem Phys Lett,1994,227:211-214
20 Greathouse JA,Cygan RT.Phys Chem Chem Phys,2005,7:3580-3586
21 Kerisit S,Liu C.Environ Sci Technol,2009,43:777-782
22 Robinson RA,Stokes RH.Electrolyte Solutions.London:Butterworth,1955