Poisson-Boltzmann与Donnan模型计算压实膨润土孔隙水与外部溶液间离子平衡的差异性比较

引用本文: 田文宇, 刘晓宇, 黎春, 王路化, 郑仲, 刘春立. Poisson-Boltzmann与Donnan模型计算压实膨润土孔隙水与外部溶液间离子平衡的差异性比较[J]. 物理化学学报, 2013, 29(06): 1209-1218. doi: 10.3866/PKU.WHXB201304031 shu

Citation: TIAN Wen-Yu, LIU Xiao-Yu, LI Chun, WANG Lu-Hua, ZHENG Zhong, LIU Chun-Li. Comparison of the Poisson-Boltzmann and Donnan Models for Calculating the Ion Equilibrium between Compacted Bentonite Porewater and External Solution[J]. Acta Physico-Chimica Sinica, 2013, 29(06): 1209-1218. doi: 10.3866/PKU.WHXB201304031 shu

Poisson-Boltzmann与Donnan模型计算压实膨润土孔隙水与外部溶液间离子平衡的差异性比较

基金项目:
国家自然科学基金(11075006, 91026010) (11075006, 91026010)

核设施退役和放射性废物治理科研专项(科工计[2007]840 号, [2012]851 号)资助项目 (科工计[2007]840 号, [2012]851 号)

摘要:

压实膨润土孔隙水与外部溶液之间的离子平衡是影响离子在压实膨润土中扩散的影响因素之一, 表征这一平衡的离子平衡系数可用压实膨润土的宏观属性参数通过Donnan 模型计算得到. 通过对膨润土主体矿物蒙脱石的TOT层结构单元进行简化, 构建了一个压实膨润土的单类孔隙结构模型, 辅以一个尺度变量H, 用Poisson-Boltzmann (PB)理论模型计算上述离子平衡系数. 对比计算结果, 发现PB模型计算的离子平衡系数总是大于Donnan模型的结果, 而参数H是联系这两种模型之间的桥梁. 通过对参数H取极限H→0, 实现了从PB模型到Donnan 模型的数学变换, 并从机理上讨论了两种模型之间的差异及其在实际扩散问题中的应用.分析表明PB模型更符合离子在压实膨润土中扩散的实际情况, 更适于处理实际扩散问题.

关键词:

English

Comparison of the Poisson-Boltzmann and Donnan Models for Calculating the Ion Equilibrium between Compacted Bentonite Porewater and External Solution

1.
Beijing National Laboratory for Molecular Sciences, Radiochemistry and Radiation Chemistry Key Laboratory for Fundamental Science, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China
Received Date: 29 January 2013
Available Online: 17 May 2013
Fund Project:
国家自然科学基金(11075006, 91026010)

核设施退役和放射性废物治理科研专项(科工计[2007]840 号, [2012]851 号)资助项目

Abstract:

The ion equilibrium at the interface of solution within compacted bentonite, and the external solution is an important factor influencing the diffusion of ionic species in the compacted bentonite. The ion equilibrium can be calculated by the Donnan model using macroscopic compacted bentonite parameters. By constructing a single pore type structure model for compacted bentonite, where the montmorillonite TOT-layers are depicted as a parallel array of rectangles, the ion equilibrium can also be calculated by the Poisson-Boltzmann (PB) model with a scale-defining variable H. We demonstrated that the ion equilibrium coefficients calculated by the PB model are always larger than those calculated by the Donnan model, and the models are linked by the factor H. The mathematical transition from the PB model to the Donnan model occurs in the limiting case H→0. The application of the two models to diffusion problem is also discussed, and the PB model is shown to be more realistic and suitable for solving actual diffusion problems.

Key words:

1. [1]
  
  (1) Pusch, R. Clay Min. 1992, 27 (3), 353. doi: 10.1180/claymin.1992.027.3.08
  (1) Pusch, R. Clay Min. 1992, 27 (3), 353. doi: 10.1180/claymin.1992.027.3.08
2. [2]
  (2) Pusch, R. Geological Storage of Highly Radioactive Waste:Current Concepts and Plans for Radioactive Waste Disposal;Springer: Berlin, 2008; p 379.(2) Pusch, R. Geological Storage of Highly Radioactive Waste:Current Concepts and Plans for Radioactive Waste Disposal;Springer: Berlin, 2008; p 379.
3. [3]
  (3) Bradbury, M. H.; Baeyens, B. J. Contam. Hydrol. 2003, 61 (1-4), 329. doi: 10.1016/S0169-7722(02)00125-0(3) Bradbury, M. H.; Baeyens, B. J. Contam. Hydrol. 2003, 61 (1-4), 329. doi: 10.1016/S0169-7722(02)00125-0
4. [4]
  (4) Overbeek, J. T. G. Prog. Biophys. Biophys. Chem. 1956, 6, 58.(4) Overbeek, J. T. G. Prog. Biophys. Biophys. Chem. 1956, 6, 58.
5. [5]
  (5) Basser, P. J.; Grodzinsky, A. J. Biophys. Chem. 1993, 46 (1), 57.doi: 10.1016/0301-4622(93)87007-J(5) Basser, P. J.; Grodzinsky, A. J. Biophys. Chem. 1993, 46 (1), 57.doi: 10.1016/0301-4622(93)87007-J
6. [6]
  (6) Dähnert, K.; Huster, D. J. Colloid Interface Sci. 1999, 215 (1),131. doi: 10.1006/jcis.1999.6238(6) Dähnert, K.; Huster, D. J. Colloid Interface Sci. 1999, 215 (1),131. doi: 10.1006/jcis.1999.6238
7. [7]
  (7) Birgersson, M.; Karnland, O. Geochim. Cosmochim. Acta 2009,73 (7), 1908. doi: 10.1016/j.gca.2008.11.027(7) Birgersson, M.; Karnland, O. Geochim. Cosmochim. Acta 2009,73 (7), 1908. doi: 10.1016/j.gca.2008.11.027
8. [8]
  (8) Boving, T. B.; Grathwohl, P. J. Contam. Hydrol. 2001, 53 (1-2),85. doi: 10.1016/S0169-7722(01)00138-3(8) Boving, T. B.; Grathwohl, P. J. Contam. Hydrol. 2001, 53 (1-2),85. doi: 10.1016/S0169-7722(01)00138-3
9. [9]
  (9) Jardat, M.; Dufreche, J. F.; Marry, V.; Rotenberg, B.; Turq, P.Phys. Chem. Chem. Phys. 2009, 11 (12), 2023. doi: 10.1039/b818055e(9) Jardat, M.; Dufreche, J. F.; Marry, V.; Rotenberg, B.; Turq, P.Phys. Chem. Chem. Phys. 2009, 11 (12), 2023. doi: 10.1039/b818055e
10. [10]
  (10) McBride, M. B. Environmental Chemistry of Soils; OxfordUniversity Press: New York, 1994; p 406.(10) McBride, M. B. Environmental Chemistry of Soils; OxfordUniversity Press: New York, 1994; p 406.
11. [11]
  (11) Van Loon, L. R.; Glaus, M. A.; Müller,W. Appl. Geochem.2007, 22 (11), 2536. doi: 10.1016/j.apgeochem.2007.07.008(11) Van Loon, L. R.; Glaus, M. A.; Müller,W. Appl. Geochem.2007, 22 (11), 2536. doi: 10.1016/j.apgeochem.2007.07.008
12. [12]
  (12) Muurinen, A.; Penttilä-Hiltunen, P.; Uusheimo, K. Mater. Res.Soc. Symp. Proc. 1989, 127, 743.(12) Muurinen, A.; Penttilä-Hiltunen, P.; Uusheimo, K. Mater. Res.Soc. Symp. Proc. 1989, 127, 743.
13. [13]
  (13) Ishidera, T.; Miyamoto, S.; Sato, H. J. Nucl. Sci. Tech. 2008, 45 (7), 610. doi: 10.3327/jnst.45.610(13) Ishidera, T.; Miyamoto, S.; Sato, H. J. Nucl. Sci. Tech. 2008, 45 (7), 610. doi: 10.3327/jnst.45.610
14. [14]
  (14) Oscarson, D.W.; Hume, H. B.; Sawatsky, N. G.; Cheung, S. C.H. Soil Sci. Soc. Am. J. 1992, 56 (5), 1400. doi: 10.2136/sssaj1992.03615995005600050011x(14) Oscarson, D.W.; Hume, H. B.; Sawatsky, N. G.; Cheung, S. C.H. Soil Sci. Soc. Am. J. 1992, 56 (5), 1400. doi: 10.2136/sssaj1992.03615995005600050011x
15. [15]
  (15) Choi, J.W.; Oscarson, D.W. J. Cont. Hydrol. 1996, 22 (3-4),189. doi: 10.1016/0169-7722(95)00081-X(15) Choi, J.W.; Oscarson, D.W. J. Cont. Hydrol. 1996, 22 (3-4),189. doi: 10.1016/0169-7722(95)00081-X
16. [16]
  (16) Kozaki, T.; Saito, N.; Fujishima, A.; Sato, S.; Ohashi, H.J. Cont. Hydrol. 1998, 35 (1-3), 67. doi: 10.1016/S0169-7722(98)00116-8(16) Kozaki, T.; Saito, N.; Fujishima, A.; Sato, S.; Ohashi, H.J. Cont. Hydrol. 1998, 35 (1-3), 67. doi: 10.1016/S0169-7722(98)00116-8
17. [17]
  (17) Kozaki, T.; Inada, K.; Sato, S.; Ohashi, H. J. Cont. Hydrol.2001, 47 (2-4), 159. doi: 10.1016/S0169-7722(00)00146-7(17) Kozaki, T.; Inada, K.; Sato, S.; Ohashi, H. J. Cont. Hydrol.2001, 47 (2-4), 159. doi: 10.1016/S0169-7722(00)00146-7
18. [18]
  (18) Molera, M.; Eriksen, T.; Jansson, M. Appl. Clay Sci. 2003, 23 (1-4), 69. doi: 10.1016/S0169-1317(03)00088-7(18) Molera, M.; Eriksen, T.; Jansson, M. Appl. Clay Sci. 2003, 23 (1-4), 69. doi: 10.1016/S0169-1317(03)00088-7
19. [19]
  (19) Peng, B.; Yu, Y. X. J. Chem. Phys. 2009, 131, 134703.doi: 10.1063/1.3243873(19) Peng, B.; Yu, Y. X. J. Chem. Phys. 2009, 131, 134703.doi: 10.1063/1.3243873
20. [20]
  (20) Yu, Y. X.;Wu, J. Z.; Gao, G. H. Chin. J. Chem. Eng. 2004,12 (5), 688.(20) Yu, Y. X.;Wu, J. Z.; Gao, G. H. Chin. J. Chem. Eng. 2004,12 (5), 688.
21. [21]
  (21) Bhuiyan, L. B.; Outhwaite, C.W. J. Chem. Phys. 2002, 116,2650. doi: 10.1063/1.1433665
  (21) Bhuiyan, L. B.; Outhwaite, C.W. J. Chem. Phys. 2002, 116,2650. doi: 10.1063/1.1433665

扫一扫看文章

计量

PDF下载量: 608
文章访问数: 1099
HTML全文浏览量: 41

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Poisson-Boltzmann与Donnan模型计算压实膨润土孔隙水与外部溶液间离子平衡的差异性比较

English

Comparison of the Poisson-Boltzmann and Donnan Models for Calculating the Ion Equilibrium between Compacted Bentonite Porewater and External Solution

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Poisson-Boltzmann与Donnan模型计算压实膨润土孔隙水与外部溶液间离子平衡的差异性比较

English

Comparison of the Poisson-Boltzmann and Donnan Models for Calculating the Ion Equilibrium between Compacted Bentonite Porewater and External Solution

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs