Trapping Cations in Specific Positions in Tuneable "Artificial Cell" Channels: New Nanochemistry Perspectives

Angewandte Chemie - International Edition

Volumn 42, Issue 41, 2003, Pages 5039-5044

  Müller, Achim ^a   Das, Samar K ^a   Talismanov, Sergei ^a   Roy, Soumyajit ^a   Beckmann, Eike ^a   Bögge, Hartmut ^a   Schmidtmann, Marc ^a   Merca, Alice ^a   Berkle, Alois ^a   Allouche, Lionel ^a   Zhou, Yunshan ^a   Zhang, Lijuan ^a  

^a BIELEFELD UNIVERSITY   (Germany)

Author keywords

Confined geometries; Encapsulation; Ion transport uptake; Nanotechnology; Porous materials

Indexed keywords

CHROMATOGRAPHIC ANALYSIS; DECISION MAKING; NANOTECHNOLOGY;

CATION TRAPPING;

POSITIVE IONS;

CATION;

ARTICLE; CATION TRANSPORT; CELL; CHEMISTRY; CHROMATOGRAPHY; FILTER; NANOPARTICLE; NANOTECHNOLOGY; POROSITY; REACTION ANALYSIS; STRUCTURE ANALYSIS;

EID: 0242291914     PISSN: 14337851     EISSN: None     Source Type: Journal    
DOI: 10.1002/anie.200352358     Document Type: Article

References (32)

1. a) Handbook of Porous Solids (Eds.: F. Schüth, K. S. W. Sing, J. Weitkamp), Wiley-VCH, Weinheim, 2002;
2. b) M. A. White, Properties of Materials, Oxford University Press, New York, 1999, chap.: Inclusion Compounds;
3. c) G. Férey, Science 2001, 291, 994-995.
4. a) A. Müller, E. Krickemeyer, H. Bögge, M. Schmidtmann, B. Botar, M. O. Talismanova, Angew. Chem. 2003, 115, 2131-2136; Angew. Chem. Int. Ed. 2003, 42, 2085-2090;
5. a) A. Müller, E. Krickemeyer, H. Bögge, M. Schmidtmann, B. Botar, M. O. Talismanova, Angew. Chem. 2003, 115, 2131-2136; Angew. Chem. Int. Ed. 2003, 42, 2085-2090;
6. b) A. Müller, E. Krickemeyer, H. Bögge, M. Schmidtmann, F. Peters, Angew. Chem. 1998, 110, 3567-3571; Angew. Chem. Int. Ed. 1998, 37, 3360-3363.
7. b) A. Müller, E. Krickemeyer, H. Bögge, M. Schmidtmann, F. Peters, Angew. Chem. 1998, 110, 3567-3571; Angew. Chem. Int. Ed. 1998, 37, 3360-3363.
8. a) A. Müller, P. Kögerler, C. Kuhlmann, Chem. Commun. 1999, 1347-1358;
9. 9) rings, are opened slightly during uptake. Related solution NMR studies concerning the stability and reaction pathways are currently possible and are in progress (F. Taulelle, M. Henry, A. Müller; see also ref. [5]).
10. See also related discussion in: M. Gross, Chem. Br. 2003, 39 (August Issue), p. 18. As the cations entering through the gates are not randomly distributed in the cell interior but fixed at functionalities according to their specific properties, thus relatively reducing the whole capsule system entropy, a situation results that is formally comparable to that of "Maxwell's Demon", but acting in a closed system (the related Gedanken experiment is for instance explained in textbooks of Statistical Thermodynamics and even in The New Encyclopaedia Britannica, Vol. 23, 15th ed., Encyclopaedia Britannica, Chicago, 2002, p. 692, including the statement: "The hypothetical intelligent being known as Maxwell's demon was a factor in the development of information theory"). See also: M. Gross, Travels to the Nanoworld: Miniature Machinery in Nature and Technology, Perseus Publishing, Cambridge, Massachusetts, 2001 (Chapter: Maxwell's demon-a predecessor of nanotechnology?); D. E. H. Jones, Nature 1995, 374, 835-837.
11. See also related discussion in: M. Gross, Chem. Br. 2003, 39 (August Issue), p. 18. As the cations entering through the gates are not randomly distributed in the cell interior but fixed at functionalities according to their specific properties, thus relatively reducing the whole capsule system entropy, a situation results that is formally comparable to that of "Maxwell's Demon", but acting in a closed system (the related Gedanken experiment is for instance explained in textbooks of Statistical Thermodynamics and even in The New Encyclopaedia Britannica, Vol. 23, 15th ed., Encyclopaedia Britannica, Chicago, 2002, p. 692, including the statement: "The hypothetical intelligent being known as Maxwell's demon was a factor in the development of information theory"). See also: M. Gross, Travels to the Nanoworld: Miniature Machinery in Nature and Technology, Perseus Publishing, Cambridge, Massachusetts, 2001 (Chapter: Maxwell's demon-a predecessor of nanotechnology?); D. E. H. Jones, Nature 1995, 374, 835-837.
12. See also related discussion in: M. Gross, Chem. Br. 2003, 39 (August Issue), p. 18. As the cations entering through the gates are not randomly distributed in the cell interior but fixed at functionalities according to their specific properties, thus relatively reducing the whole capsule system entropy, a situation results that is formally comparable to that of "Maxwell's Demon", but acting in a closed system (the related Gedanken experiment is for instance explained in textbooks of Statistical Thermodynamics and even in The New Encyclopaedia Britannica, Vol. 23, 15th ed., Encyclopaedia Britannica, Chicago, 2002, p. 692, including the statement: "The hypothetical intelligent being known as Maxwell's demon was a factor in the development of information theory"). See also: M. Gross, Travels to the Nanoworld: Miniature Machinery in Nature and Technology, Perseus Publishing, Cambridge, Massachusetts, 2001 (Chapter: Maxwell's demon-a predecessor of nanotechnology?); D. E. H. Jones, Nature 1995, 374, 835-837.
13. See also related discussion in: M. Gross, Chem. Br. 2003, 39 (August Issue), p. 18. As the cations entering through the gates are not randomly distributed in the cell interior but fixed at functionalities according to their specific properties, thus relatively reducing the whole capsule system entropy, a situation results that is formally comparable to that of "Maxwell's Demon", but acting in a closed system (the related Gedanken experiment is for instance explained in textbooks of Statistical Thermodynamics and even in The New Encyclopaedia Britannica, Vol. 23, 15th ed., Encyclopaedia Britannica, Chicago, 2002, p. 692, including the statement: "The hypothetical intelligent being known as Maxwell's demon was a factor in the development of information theory"). See also: M. Gross, Travels to the Nanoworld: Miniature Machinery in Nature and Technology, Perseus Publishing, Cambridge, Massachusetts, 2001 (Chapter: Maxwell's demon-a predecessor of nanotechnology?); D. E. H. Jones, Nature 1995, 374, 835-837.
14. Both are formed by ligand exchange from 3a, which is available in facile syntheses according to: L. Cronin, E. Diemann, A. Müller in Inorganic Experiments (Ed.: J. D. Woollins), 2nd ed., Wiley-VCH, Weinheim, 2003, pp. 340-346 and A. Müller, S. K. Das, E. Krickemeyer, C. Kuhlmann, Inorg. Synth. 2003, 34, in press. The sulfate cluster anion 1a[2a] with the high charge of 72-is formed from 3a in situ in solution during the processes leading to 4a, 5a, and 6a, which can also be obtained by starting from solutions of crystalline 1. Important in context with footnote [3] is that 1a can be obtained by ligand exchange from 3a without heating, that is at room temperature and under low pH conditions which supports the release of the leaving group acetic acid.
15. Both are formed by ligand exchange from 3a, which is available in facile syntheses according to: L. Cronin, E. Diemann, A. Müller in Inorganic Experiments (Ed.: J. D. Woollins), 2nd ed., Wiley-VCH, Weinheim, 2003, pp. 340-346 and A. Müller, S. K. Das, E. Krickemeyer, C. Kuhlmann, Inorg. Synth. 2003, 34, in press. The sulfate cluster anion 1a[2a] with the high charge of 72-is formed from 3a in situ in solution during the processes leading to 4a, 5a, and 6a, which can also be obtained by starting from solutions of crystalline 1. Important in context with footnote [3] is that 1a can be obtained by ligand exchange from 3a without heating, that is at room temperature and under low pH conditions which supports the release of the leaving group acetic acid.
16. Ka radiation, graphite monochromator; hemisphere data collection in ω at 0.3° scan width in three runs with 606, 435, and 230 frames (φ = 0, 88, and 180°) at a detector distance of 4.0-5.0 cm). For all structures empirical absorption corrections were performed by using equivalent reflections with the program SADABS 2.03. The structures were solved with the program SHELXS-97 and refined by using SHELXL-93. (SHELXS/L, SADABS from G. M. Sheldrick, University of Göttingen (Germany) 1993/97; structure graphics with DIAMOND 2.1 from K. Brandenburg, Crystal Impact GbR, 2001). Further details of the crstal structure investigations can be obtained from the Fachinformationszentrum Karlsruhe, 76344 Eggenstein-Leopoldshafen, Germany, (fax: (+49)7247-808-666; e-mail: crysdata@fiz.karlsruhe.de) on quoting the depository numbers CSD-413 251 (2), CSD 413 252 (4), CSD 413 253 (5), CSD 413 254 (6) and CSD 413 255 (7).
17. Ka radiation, graphite monochromator; hemisphere data collection in ω at 0.3° scan width in three runs with 606, 435, and 230 frames (φ = 0, 88, and 180°) at a detector distance of 4.0-5.0 cm). For all structures empirical absorption corrections were performed by using equivalent reflections with the program SADABS 2.03. The structures were solved with the program SHELXS-97 and refined by using SHELXL-93. (SHELXS/L, SADABS from G. M. Sheldrick, University of Göttingen (Germany) 1993/97; structure graphics with DIAMOND 2.1 from K. Brandenburg, Crystal Impact GbR, 2001). Further details of the crstal structure investigations can be obtained from the Fachinformationszentrum Karlsruhe, 76344 Eggenstein-Leopoldshafen, Germany, (fax: (+49)7247-808-666; e-mail: crysdata@fiz.karlsruhe.de) on quoting the depository numbers CSD-413 251 (2), CSD 413 252 (4), CSD 413 253 (5), CSD 413 254 (6) and CSD 413 255 (7).
18. 31P MAS NMR spectra allow us to distinguish between the "phosphates" coordinated as ligands and those abundant in the crystal lattice.
19. A. Müller, E. Krickemeyer, H. Bögge, M. Schmidtmann, S. Roy, A. Berkle, Angew. Chem. 2002, 114, 3756-3761; Angew. Chem. Int. Ed. 2002, 41, 3604-3609.
20. A. Müller, E. Krickemeyer, H. Bögge, M. Schmidtmann, S. Roy, A. Berkle, Angew. Chem. 2002, 114, 3756-3761; Angew. Chem. Int. Ed. 2002, 41, 3604-3609.
21. J.-M. Lehn, Supramolecular Chemistry: Concepts and Perspectives, VCH, Weinheim, 1995, p. 28.
22. For the transport of the cations through biological membranes, negatively charged amino acids play a key role; see: D. Voet, J. G. Voet, Biochemistry, 2nd ed., Wiley, New York, 1995, chap. 18.
23. 3H). As three pentagonal faces are connected at each vertex this leads to a total number of 8 = (12 × 2)/3 positions; see Figure 3).
24. For related topics see: a) K. E. Drexler, Nanosystems: Molecular Machinery, Manufacturing, and Computation, Wiley, New York, 1992;
25. b) Recent Advances in the Chemistry of Nanomaterials (Eds.: C. N. R. Rao, A. Müller, A. K. Cheetham), Wiley-VCH, Weinheim, in press;
26. c) P. Ball, Made to Measure: New Materials for the 21st Century, Princeton University Press, Princeton, 1997;
27. regarding the importance of pores see also: d) J. Tersoff, Nature 2001, 412, 135-136.
28. 3+).
29. The phenomenon of trapping aqueous solutes/complexes will be studied separately: A. Müller, Y. Zhou, L. Zhang, L. Toma, H. Bögge, M. Schmidtmann, unpublished results.
30. A. F. Voegele, K. R. Liedl, Angew. Chem. 2003, 115, 2162-2164; Angew. Chem. Int. Ed. 2003, 42, 2114-2116.
31. A. F. Voegele, K. R. Liedl, Angew. Chem. 2003, 115, 2162-2164; Angew. Chem. Int. Ed. 2003, 42, 2114-2116.
32. Note added in proof (Setember 24, 2003): According to new NMR investigations (F. Taulelle, M. Henry, A. Müller) the stability of the capsule in solution is very high. Furthermore the exchange of the acetate ligands of the starting material 3a is easily possible under low pH conditions (see also ref. [5]).