Diluting the hydrogen bonds in viscous solutions of n -butanol with n -bromobutane: A dielectric study

Journal of Chemical Physics

Volumn 128, Issue 15, 2008, Pages

  El Goresy, T ^a   Bohmer R ^a  

^a TU DORTMUND UNIVERSITY   (Germany)

Author keywords

[No Author keywords available]

Indexed keywords

BROMINE COMPOUNDS; BUTANE; BUTENES; DIELECTRIC PROPERTIES; DILUTION; GLASS TRANSITION; HYDROGEN BONDS; STRUCTURAL RELAXATION; VISCOUS FLOW;

BROMOBUTANES; DEBYE RELAXATION; DECOUPLINGS; GLASS FORMING MONOHYDROXY ALCOHOLS; SPECTRAL BROADENING; VISCOUS SOLUTIONS;

ALCOHOLS;

EID: 42449104945     PISSN: 00219606     EISSN: None     Source Type: Journal    
DOI: 10.1063/1.2903403     Document Type: Article

References (45)

1. See, e.g., P. Lunkenheimer, R. Wehn, U. Schneider, and A. Loidl, Phys. Rev. Lett. 95, 055702 (2005).
2. K. Schmidt-Rohr and H. W. Spiess, Phys. Rev. Lett. 66, 3020 (1991).
3. See, e.g., L.-M. Wang and R. Richert, J. Chem. Phys. 123, 054516 (2005), and references cited therein.
4. R. Wassink and P. Bordewijk, Adv. Mol. Relax. Interact. Processes 0378-4487 10.1016/0378-4487(78)80051-X 13, 299 (1978); A. K. Karmaker, S. Sarkar, and R. N. Joarder, J. Phys. Chem. 0022-3654 10.1021/j100045a001 99, 16501 (1995); S. W. Benson, J. Am. Chem. Soc. 0002-7863 10.1021/ja962101w 118, 10645 (1996); A. K. Sum and S. I. Sandler, J. Phys. Chem. A 104, 1121 (2000).
5. M. A. Floriano and C. A. Angell, J. Chem. Phys. 91, 2537 (1989).
6. H. Huth, L.-M. Wang, C. Schick, and R. Richert, J. Chem. Phys. 126, 104503 (2007).
7. A. Schallamach, Trans. Faraday Soc. 42, A180 (1946).
8. D. J. Denney, J. Chem. Phys. 30, 1019 (1959).
9. P. Daumezon and R. Heitz, J. Chem. Phys. 55, 5704 (1971).
10. S. S. N. Murthy and M. Tyagi, J. Chem. Phys. 117, 3837 (2002).
11. G. Power, J. K. Vij, and G. P. Johari, J. Chem. Phys. 0021-9606 10.1063/1.2409929 126, 034512 (2007); G. Power, J. K. Vij, and G. P. Johari, J. Chem. Phys. 127, 094507 (2007).
12. S. S. N. Murthy, J. Sobhanadri, and Gangasharan, J. Chem. Phys. 100, 4601 (1994).
13. W. Dannhauser and R. H. Cole, J. Chem. Phys. 23, 1762 (1955).
14. S. S. N. Murthy and S. K. Nayak, J. Chem. Phys. 99, 5362 (1993).
15. B. V. Bolshakov and A. G. Dzhonson, Dokl. Phys. Chem. 0012-5016 10.1023/B:DOPC.0000003470.16468.dc 393, 318 (2003); B. V. Bolshakov and A. G. Dzhonson, J. Non-Cryst. Solids 351, 444 (2005).
16. R. Kurita and H. Tanaka, J. Phys.: Condens. Matter 17, L293 (2005); These authors suggest that liquid-liquid transitions may be facilitated in molecular liquids "which have a tendency to form long-lived locally favored structures due to anisotropic interactions (e.g., hydrogen bonding)."
17. L.-M. Wang, S. Shahriari, and R. Richert, J. Phys. Chem. B 109, 23255 (2005).
18. N. B. Olsen, personal communication (29 June 2007).
19. A. Ansón, R. Garriga, S. Martínez, P. Ṕrez, and M. Gracia, J. Chem. Eng. Data 50, 1478 (2005) report densities ρ BuBr =1.266 83 g cm3 and of ρ BuOH =0.805 40 g cm3 at 298.15 K. In Eq., the number density n=ρ NA Mmol is required with NA denoting Avogadro's constant and Mmol denoting the molecular mass. Thus, the proper ratio is (n μ2 Tmax)BuBr (n μ2 Tmax)BuOH ≈1.55 with Tmax designating the temperature at which the data shown in Fig. were obtained. For 318.15 K, A. Ansón, report a maximum of the excess molar volume of 0.3 cm3 mol near x=40%.
20. A. Loidl, T. Schräder, R. Böhmer, K. Knorr, J. K. Kjems, and R. Born, Phys. Rev. B 34, 1238 (1986).
21. L.-M. Wang and R. Richert, J. Phys. Chem. B 109, 8767 (2005).
22. R. Böhmer, K. L. Ngai, C. A. Angell, and D. J. Plazek, J. Chem. Phys. 99, 4201 (1993).
23. C. A. Angell, Chem. Rev. (Washington, D.C.) 90, 523 (1990).
24. F. Qi, R. Böhmer, and H. Sillescu, Phys. Chem. Chem. Phys. 3, 4022 (2001).
25. While the present article is focused on the low-temperature end of the viscous regime, L.-M. Wang and R. Richert, J. Chem. Phys. 121, 11170 (2004) pointed out that at high temperatures, a τD τα ratio of about 100 is attained for many monohydroxy alcohols.
26. The notion of dynamic clusters in relation to percolation phenomena in supercooled liquids and other disordered systems has been used, e.g., by R. V. Chamberlin and D. N. Haines, Phys. Rev. Lett. 0031-9007 10.1103/PhysRevLett.65. 2197 65, 2197 (1990); R. V. Chamberlin, R. Böhmer, E. Sanchez, and C. A. Angell, Phys. Rev. B 46, 5787 (1992).
27. The familiar conjecture that "the primary alcohols are associated into chains of great length," with the specification "these chains are very stable," from A. V. Lesikar, J. Solution Chem. 6, 839 (1977), seems hard to reconcile with the fact that these "chains" apparently do not have a detectable impact on the mechanical stability given the long-time scales associated with the Debye process relative to that of the α relaxation.
28. This should not be read to imply that H-bond induced clustering or multimer formation [see, e.g., L. Stordrange, A. A. Christy, O. M. Kvalheim, H. Shen, and Y. Liang, J. Phys. Chem. A 1089-5639 10.1021/jp013670f 106, 8543 (2002)] is generally unobservable. In the supercooled liquid state, it has been seen in neutron scattering via a structure factor prepeak, e.g., for meta-fluoroaniline [D. Morineau, C. Alba-Simionesco, M. C. Bellissent-Funel, and M.-F. Lauthí, Europhys. Lett. 0295-5075 10.1209/epl/i1998-00339-6 43, 195 (1998)]. This hydrogen-bonded substance, however, does not exhibit Debye-like features in its dielectric response [A. Kudlik, C. Tschirwitz, S. Benkhof, T. Blochowicz, and E. Rössler, Europhys. Lett. 40, 649 (1997)].
29. W. Huang and R. Richert, J. Chem. Phys. 124, 164510 (2006).
30. R. Kono, T. A. Litovitz, and G. E. McDuffie, J. Chem. Phys. 45, 1790 (1966).
31. M. T. Cicerone, F. R. Blackburn, and M. D. Ediger, J. Chem. Phys. 102, 471 (1995).
32. L.-M. Wang and R. Richert, J. Chem. Phys. 120, 11082 (2004).
33. This is why we refrain from the designation α′ which has been occasionally used for Debye-like processes and other processes of unclear origin which are slower than the α relaxation. The designation α′ was suggested, e.g., in Ref. or in D. L. Sidebottom, R. Bergman, L. Börjesson, and L. M. Torell, Phys. Rev. Lett. 0031-9007 10.1103/PhysRevLett.68.3587 68, 3587 (1992); H. Kriegs, J. Gapinski, G. Meier, M. Paluch, S. Pawlus, and A. Patkowski, J. Chem. Phys. 124, 104901 (2006).
34. N. G. McCrum, B. E. Read, and G. Williams, Anelastic and Dielectric Effects in Polymeric Solids (Wiley, New York, 1967).
35. S. S. N. Murthy, Gangasharan, and S. K. Nayak, J. Chem. Soc., Faraday Trans. 89, 509 (1993).
36. T. A. Litovitz and G. E. McDuffie, Jr., J. Chem. Phys. 0021-9606 10.1063/1.1734316 39, 723 (1963); V. A. Solovyev, C. J. Montrose, M. H. Watkins, and T. A. Litovitz, J. Chem. Phys. 48, 2155 (1968).
37. H. Versmold, Ber. Bunsenges. Phys. Chem. 0005-9021 78, 1318 (1974); H. G. Hertz, T. Wild, and H. Weingärtner, Z. Phys. Chem. 0942-9352 140, 71 (1984); R. Ludwig, M. D. Zeidler, and T. C. Farrar, Z. Phys. Chem. 189, 19 (1995).
38. M. Pöschl and H. G. Hertz, J. Phys. Chem. 98, 8195 (1994).
39. Room temperature data were reported by H. Nadolny, A. Volmari, and H. Weingärtner, Ber. Bunsenges. Phys. Chem. 102, 866 (1998).
40. B. Schiener and R. Böhmer, J. Non-Cryst. Solids 182, 180 (1995).
41. C. Hansen, F. Stickel, T. Berger, R. Richert, and E. W. Fischer, J. Chem. Phys. 107, 1086 (1997).
42. D. W. Davidson, Can. J. Chem. 39, 2139 (1961).
43. H. Mandal and S. Walker, Z. Phys. Chem. 165, 119 (1989).
44. G. P. Johari, O. E. Kalinovskaya, and J. K. Vij, J. Chem. Phys. 114, 4634 (2001).
45. CRC Handbook of Chemistry and Physics, 79th ed., edited by, D. R. Lide, (Chemical Rubber, Cleveland, 1998), pp. 9-43.