NO<sub>x</sub>分子在[Ag]-MAPO-5 (M=Si, Ti) 分子筛中的吸附

引用本文: 刘洁翔, 张晓光, 段中余, 刘晓莉. NO_x分子在[Ag]-MAPO-5 (M=Si, Ti) 分子筛中的吸附[J]. 物理化学学报, 2010, 26(10): 2679-2685. doi: 10.3866/PKU.WHXB20101013 shu

Citation: LIU Jie-Xiang, ZHANG Xiao-Guang, DUAN Zhong-Yu, LIU Xiao-Li. NO_x Molecule Adsorption in [Ag]-MAPO-5 (M=Si, Ti)Molecular Sieves[J]. Acta Physico-Chimica Sinica, 2010, 26(10): 2679-2685. doi: 10.3866/PKU.WHXB20101013 shu

NO_x分子在[Ag]-MAPO-5 (M=Si, Ti) 分子筛中的吸附

基金项目:
河北省科技支撑计划(06215124) (06215124)

天津市自然科学基金(08JCYBJC00700)资助项目. (08JCYBJC00700)

摘要:

采用密度泛函理论(DFT) 研究了银离子交换的硅磷酸铝([Ag]-SAPO-5)和钛磷酸铝([Ag]-TAPO-5)分子筛结构及其对NO_x 分子的吸附, 获得吸附复合物的平衡几何结构参数和吸附能. 结果表明, NO_x 分子以η¹-N 模式吸附在[Ag]-SAPO-5 和[Ag]-TAPO-5 分子筛中的结构更稳定, 其吸附作用强度的次序为NO₂>NO>N₂O.[Ag]-SAPO-5 和[Ag]-TAPO-5 对NO 和NO₂ 分子的活化程度要比N₂O 大. 相比[Ag]-AlMOR,[Ag]-SAPO-5 和[Ag]-TAPO-5 对NO_x 分子的活化程度较大. 还对[Ag]-SAPO-5 和[Ag]-TAPO-5 分子筛的抗硫、抗水及抗氧化性能进行了研究和分析. 另外, 通过自然键轨道(NBO) 计算, 分析了NO_x 分子与平衡离子Ag⁺之间的作用机理.

关键词:

English

NO_x Molecule Adsorption in [Ag]-MAPO-5 (M=Si, Ti)Molecular Sieves

1.
1. School of Chemical Engineering, Hebei University of Technology, Tianjin 300130, P. R. China;
2. College of Chemistry, Nankai University, Tianjin 300071, P. R. China
Received Date: 20 April 2010
Available Online: 27 September 2010
Fund Project:
河北省科技支撑计划(06215124)

天津市自然科学基金(08JCYBJC00700)资助项目.

Abstract:

NO_x adsorption in silver-exchanged aluminophosphate molecular sieves ([Ag]-SAPO-5 and [Ag]-TAPO-5) was investigated using the density functional theory (DFT). Equilibrium structure parameters and adsorption energies were obtained and compared. The results indicated that the η¹-N mode was more stable than the η¹-O mode. The adsorption energy values of NO_x followed the order: NO₂>NO>N₂O. Compared to the free gas state, the bond parameters of NO and NO₂ in the adsorbed state changed more than that of N₂O in [Ag]-SAPO-5 and [Ag]-TAPO-5. Moreover, [Ag]-SAPO-5 and [Ag]-TAPO-5 had a higher activation for the NO_x molecule compared to [Ag]-AlMOR. The resistance capabilities of [Ag]-SAPO-5 and [Ag]-TAPO-5 to SO₂,H₂O, and O₂ were also studied and analyzed. In addition, the interaction mechanism of NO_x in silver-exchanged aluminophosphate molecular sieves was investigated using natural bond orbital (NBO) analysis.

Key words:

1. [1]
  
  1. Iwamoto, M.; Furukawa, H.; Kagawa, S. Newdevelopments in zeolite science and technology. Amsterdam: Elsevier, 1986: 943
  1. Iwamoto, M.; Furukawa, H.; Kagawa, S. Newdevelopments in zeolite science and technology. Amsterdam: Elsevier, 1986: 943
2. [2]
  2. Sun, Y. M.; Yang, P.; Cao, A. N.; Zhang, Y. Acta Phys.-Chim. Sin., 2001, 17(8): 761 [孙岳明,杨萍,曹爱年,张远援物理化学学报, 2001, 17(8): 761]2. Sun, Y. M.; Yang, P.; Cao, A. N.; Zhang, Y. Acta Phys.-Chim. Sin., 2001, 17(8): 761 [孙岳明,杨萍,曹爱年,张远援物理化学学报, 2001, 17(8): 761]
3. [3]
  3. Feng, X. B.; Keith, H. W. J. Catal., 1997, 166: 3683. Feng, X. B.; Keith, H. W. J. Catal., 1997, 166: 368
4. [4]
  4. Iwamoto, M.; Yahiro, H.; Shin, H. K.; Watanabe, M.; Guo, J.W.; Konno, M.; Chikahisa, T.; Murayama, T. Appl. Catal. B-Environ., 1994, 5: L14. Iwamoto, M.; Yahiro, H.; Shin, H. K.; Watanabe, M.; Guo, J.W.; Konno, M.; Chikahisa, T.; Murayama, T. Appl. Catal. B-Environ., 1994, 5: L1
5. [5]
  5. Bethke, K. A.; Kung, H. H. J. Catal., 1997, 172: 935. Bethke, K. A.; Kung, H. H. J. Catal., 1997, 172: 93
6. [6]
  6. Shimizu, K. A.; Hattori, T. Appl. Catal. B-Environ., 2000, 25: 2396. Shimizu, K. A.; Hattori, T. Appl. Catal. B-Environ., 2000, 25: 239
7. [7]
  7. Shi, C.; Cheng, M. J.; Qu, Z. P.; Yang, X. F.; Bao. X. H. Chem. J. Chin. Univ., 2003, 23(4): 628 [石川,程谟杰, 曲振平,杨学锋,包信和.高等学校化学学报, 2003, 23(4): 628]7. Shi, C.; Cheng, M. J.; Qu, Z. P.; Yang, X. F.; Bao. X. H. Chem. J. Chin. Univ., 2003, 23(4): 628 [石川,程谟杰, 曲振平,杨学锋,包信和.高等学校化学学报, 2003, 23(4): 628]
8. [8]
  8. Li, Z.; Flytzani-Stephanopoulos, M. J. Catal., 1999, 182: 3138. Li, Z.; Flytzani-Stephanopoulos, M. J. Catal., 1999, 182: 313
9. [9]
  9. Masuda, K.; Shinodab, K.; Katob, T.; Tsujimura, K. Appl. Catal. B- Environ., 1998, 15: 299. Masuda, K.; Shinodab, K.; Katob, T.; Tsujimura, K. Appl. Catal. B- Environ., 1998, 15: 29
10. [10]
  10. Akolekar, D. B.; Bhargava, S. K. J. Mol. Catal. A-Chem., 2000, 157: 19910. Akolekar, D. B.; Bhargava, S. K. J. Mol. Catal. A-Chem., 2000, 157: 199
11. [11]
  11. Kurshev,V.; Kevan, L.; Parillo, D. J.; Pereira, C.; Kokotailo, G. T.; rte, R. J. J. Phys. Chem., 1994, 98: 1016011. Kurshev,V.; Kevan, L.; Parillo, D. J.; Pereira, C.; Kokotailo, G. T.; rte, R. J. J. Phys. Chem., 1994, 98: 10160
12. [12]
  12. Campelo, J. M.; Garcia, A; Luna, D.; Marinas, J. M.; Martinez, M. I. Mater. Chem. Phys., 1989, 21: 40912. Campelo, J. M.; Garcia, A; Luna, D.; Marinas, J. M.; Martinez, M. I. Mater. Chem. Phys., 1989, 21: 409
13. [13]
  13. Dědecek, J.; Cejka, J.; Wichterlová, B. Appl. Catal. B-Environ., 1998, 15: 23313. Dědecek, J.; Cejka, J.; Wichterlová, B. Appl. Catal. B-Environ., 1998, 15: 233
14. [14]
  14. Frache, A.; Palella, B.; Cadoni, M.; Pirone, R.; Ciambelli, P.; Pastore, H. O.; Marchese, L. Catal. Today, 2002, 75: 35914. Frache, A.; Palella, B.; Cadoni, M.; Pirone, R.; Ciambelli, P.; Pastore, H. O.; Marchese, L. Catal. Today, 2002, 75: 359
15. [15]
  15. Panayotov, D.; Dimitrov, L.; Khristova, M.; Petrov, L.; Mehandjiev, D. Appl. Catal. B-Environ., 1995, 6: 6115. Panayotov, D.; Dimitrov, L.; Khristova, M.; Petrov, L.; Mehandjiev, D. Appl. Catal. B-Environ., 1995, 6: 61
16. [16]
  16. Elanany, M.; Vercauteren, D. P.; Kubo, M.; Miyamoto, A. J. Mol. Catal. A-Chem., 2006, 248: 18116. Elanany, M.; Vercauteren, D. P.; Kubo, M.; Miyamoto, A. J. Mol. Catal. A-Chem., 2006, 248: 181
17. [17]
  17. Liu, J. X.;Wei, X.; Zhang, X. G.; Han, E. S. Acta Phys.-Chim. Sin., 2009, 25(10): 2123 [刘洁翔, 魏贤,张晓光,韩恩山. 物理化学学报, 2009, 25(10): 2123]17. Liu, J. X.;Wei, X.; Zhang, X. G.; Han, E. S. Acta Phys.-Chim. Sin., 2009, 25(10): 2123 [刘洁翔, 魏贤,张晓光,韩恩山. 物理化学学报, 2009, 25(10): 2123]
18. [18]
  18. Liu, J. X.;Wei, X.; Zhang, X. G.; Wang, G. X.; Han, E. S.; Wang, J. G. Acta Phys.-Chim. Sin., 2009, 25(1): 91 [刘洁翔,魏贤, 张晓光, 王桂香,韩恩山,王建国.物理化学学报, 2009, 25(1): 91]18. Liu, J. X.;Wei, X.; Zhang, X. G.; Wang, G. X.; Han, E. S.; Wang, J. G. Acta Phys.-Chim. Sin., 2009, 25(1): 91 [刘洁翔,魏贤, 张晓光, 王桂香,韩恩山,王建国.物理化学学报, 2009, 25(1): 91]
19. [19]
  19. Jiang, N.; Yuan, S. P.; Qin, Z. F.; Wang, J. G.; Jiao, H. J., Li ,Y. W. Chinese Journal of Catalysis, 2001, 25(10): 779 [蒋南,袁淑萍,秦张峰,王建国, 焦海军, 李永旺援催化学报, 2001, 25(10): 779]19. Jiang, N.; Yuan, S. P.; Qin, Z. F.; Wang, J. G.; Jiao, H. J., Li ,Y. W. Chinese Journal of Catalysis, 2001, 25(10): 779 [蒋南,袁淑萍,秦张峰,王建国, 焦海军, 李永旺援催化学报, 2001, 25(10): 779]
20. [20]
  20. Uzunova, E. L.; Göltl, F.; Kresse, G.; Hafner, J. J. Phys. Chem. C, 2009, 113: 527420. Uzunova, E. L.; Göltl, F.; Kresse, G.; Hafner, J. J. Phys. Chem. C, 2009, 113: 5274
21. [21]
  21. Material Studio, Version 2.2.1. San Die : Accehys Inc., 200221. Material Studio, Version 2.2.1. San Die : Accehys Inc., 2002
22. [22]
  22. Becke, A. D. J. Chem. Phys., 1988, 88: 254722. Becke, A. D. J. Chem. Phys., 1988, 88: 2547
23. [23]
  23. Lee, C.; Yang, W.; Parr, R. G. Phys. Rev. B-Solid State, 1988, 37: 78523. Lee, C.; Yang, W.; Parr, R. G. Phys. Rev. B-Solid State, 1988, 37: 785
24. [24]
  24. Bergner, A.; Dolg, M.; Kuechle,W.; Stoll, H.; Preuss, H. Mol. Phys., 1993, 80: 143124. Bergner, A.; Dolg, M.; Kuechle,W.; Stoll, H.; Preuss, H. Mol. Phys., 1993, 80: 1431
25. [25]
  25. Zhou, D. H.; He, N.; Wang, Y. Q.; Yang, G.; Liu, X. C.; Bao, X. H. J. Mol. Struct.-Theochem, 2005, 756: 3925. Zhou, D. H.; He, N.; Wang, Y. Q.; Yang, G.; Liu, X. C.; Bao, X. H. J. Mol. Struct.-Theochem, 2005, 756: 39
26. [26]
  26. Zhou, D. H.; Wang, Y. Q.; He, N.; Yang, G. Acta Phys.-Chim. Sin., 2006, 22(5): 512 [周丹红,王玉清,贺宁,杨刚. 物理化学学报, 2006, 22(5): 512]26. Zhou, D. H.; Wang, Y. Q.; He, N.; Yang, G. Acta Phys.-Chim. Sin., 2006, 22(5): 512 [周丹红,王玉清,贺宁,杨刚. 物理化学学报, 2006, 22(5): 512]
27. [27]
  27. Glendening, E. D.; Reed, A. E.; Carpenter, J. E.; et al. Gaussian 03, Revision B.04, NBOVersion 3.1. Pittsburgh, PA: Gaussian Inc., 200527. Glendening, E. D.; Reed, A. E.; Carpenter, J. E.; et al. Gaussian 03, Revision B.04, NBOVersion 3.1. Pittsburgh, PA: Gaussian Inc., 2005
28. [28]
  28. Zhanpeisov, N. U.; Martra, G.; Ju, W. S.; Matsuoka, M.; Coluccia, S.; Anpo, M. J. Mol. Catal. A-Chem., 2003, 201: 23728. Zhanpeisov, N. U.; Martra, G.; Ju, W. S.; Matsuoka, M.; Coluccia, S.; Anpo, M. J. Mol. Catal. A-Chem., 2003, 201: 237
29. [29]
  29. Zhang, T.; Ren, L. L.; Lin, L. W. Chinese Journal of Catalysis, 2004, 25(1): 75 [张涛, 任丽丽,林励吾援催化学报, 2004, 25 (1): 75]
  29. Zhang, T.; Ren, L. L.; Lin, L. W. Chinese Journal of Catalysis, 2004, 25(1): 75 [张涛, 任丽丽,林励吾援催化学报, 2004, 25 (1): 75]

扫一扫看文章

计量

PDF下载量: 1197
文章访问数: 4524
HTML全文浏览量: 31

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

NO_x分子在[Ag]-MAPO-5 (M=Si, Ti) 分子筛中的吸附

English

NO_x Molecule Adsorption in [Ag]-MAPO-5 (M=Si, Ti)Molecular Sieves

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

NOx分子在[Ag]-MAPO-5 (M=Si, Ti) 分子筛中的吸附

English

NOx Molecule Adsorption in [Ag]-MAPO-5 (M=Si, Ti)Molecular Sieves

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

NO_x分子在[Ag]-MAPO-5 (M=Si, Ti) 分子筛中的吸附

NO_x Molecule Adsorption in [Ag]-MAPO-5 (M=Si, Ti)Molecular Sieves

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs