BH4- Self-Diffusion in Liquid LiBH4

被引：14

作者：

Martelli, Pascal ^{[1
,2
]}

Remhof, Arndt ^{[1
]}

Borgschulte, Andreas ^{[1
]}

Mauron, Philippe ^{[1
]}

Wallacher, Dirk ^{[3
]}

Kemner, Ewout ^{[3
]}

Russina, Margarita ^{[3
]}

Pendolino, Flavio ^{[1
]}

Zuettel, Andreas ^{[1
,2
]}

机构：

[1] Empa Swiss Fed Labs Mat Sci & Technol Hydrogen &, CH-8600 Dubendorf, Switzerland

[2] Univ Fribourg, Dept Phys, CH-1700 Fribourg, Switzerland

[3] Helmholtz Zentrum Berlin, Dept Methods & Instruments, D-14109 Berlin, Germany

来源：

JOURNAL OF PHYSICAL CHEMISTRY A | 2010年 / 114卷 / 37期

基金：

瑞士国家科学基金会;

关键词：

HYDROGEN; MECHANISM; EXCHANGE; DYNAMICS; CHLORIDE;

D O I：

10.1021/jp105585h

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The hydrogen dynamics in solid and in liquid LiBH4 was studied by means of incoherent quasielastic neutron scattering. Rotational jump diffusion of the BH4- subunits on the picosecond scale was observed in solid LiBH4. The characteristic time constant is significantly shortened when the system transforms from the low-temperature phase to the high-temperature phase at 383 K. In the molten phase of LiBH4 above 553 K, translational diffusion of the BH4- units is found. The measured diffusion coefficients are in the 10(-5)cm(2)/s range at temperatures around 700 K, which is in the same order of magnitude as the self-diffusion of liquid lithium or the diffusion of ions in molten alkali halides. The temperature dependence of the diffusion coefficient shows an Arrhenius behavior, with an activation energy of E-a = 88 meV and a prefactor of D-0 = 3.1 x 10(-4)cm(2)/s.

引用

页码：10117 / 10121

页数：5

共 34 条

[1] SELF-DIFFUSION AND HETERODIFFUSION IN CRYSTALLINE SOLID-SOLUTIONS [J].

BENIERE, F ;

BENIERE, M ;

BABU, VH ;

REDDY, KV .

JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS, 1994, 55 (07) :595-604

[2] Hydrogen-deuterium exchange in bulk LiBH4 [J].

Borgschulte, A. ;

Zuettel, A. ;

Hug, P. ;

Racu, A. -M. ;

Schoenes, J. .

JOURNAL OF PHYSICAL CHEMISTRY A, 2008, 112 (21) :4749-4753

[3]

BORGSCHULTE A, 2010, Z PHYS CHEM CHEM PHY, V12, P5061

[4] SELF-DIFFUSION IN MOLTEN SODIUM CHLORIDE - A TEST OF THE APPLICABILITY OF THE NERNST-EINSTEIN EQUATION [J].

BORUCKA, AZ ;

BOCKRIS, JO ;

KITCHENER, JA .

PROCEEDINGS OF THE ROYAL SOCIETY OF LONDON SERIES A-MATHEMATICAL AND PHYSICAL SCIENCES, 1957, 241 (1227) :554-567

[5] Dynamical properties and temperature induced molecular disordering of LiBH4 and LiBD4 [J].

Buchter, F. ;

Lodziana, Z. ;

Mauron, Ph. ;

Remhof, A. ;

Friedrichs, O. ;

Borgschulte, A. ;

Zuettel, A. ;

Sheptyakov, D. ;

Straessle, Th. ;

Ramirez-Cuesta, A. J. .

PHYSICAL REVIEW B, 2008, 78 (09)

[6] Chemical and Physical Solutions for Hydrogen Storage [J].

Eberle, Ulrich ;

Felderhoff, Michael ;

Schueth, Ferdi .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2009, 48 (36) :6608-6630

[7] Introduction to Quasielastic Neutron Scattering [J].

Embs, Jan Peter ;

Juranyi, Fanni ;

Hempelmann, Rolf .

ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS, 2010, 224 (1-2) :5-32

[8] THE DIFFUSION OF LI-6 AND LI-7 AND THE ISOTOPE EFFECT IN LIQUID LITHIUM [J].

FEINAUER, A ;

MAJER, G ;

SEEGER, A .

JOURNAL OF PHYSICS-CONDENSED MATTER, 1994, 6 (26) :L355-L360

[9] Breaking the passivation-the road to a solvent free borohydride synthesis [J].

Friedrichs, O. ;

Remhof, A. ;

Borgschulte, A. ;

Buchter, F. ;

Orimo, S. I. ;

Zuettel, A. .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2010, 12 (36) :10919-10922

[10] Evidence for hydrogen transport in deuterated LiBH4 from low-temperature Raman-scattering measurements and first-principles calculations [J].

Gremaud, R. ;

Lodziana, Z. ;

Hug, P. ;

Willenberg, B. ;

Racu, A-M. ;

Schoenes, J. ;

Ramirez-Cuesta, A. J. ;

Clark, S. J. ;

Refson, K. ;

Zuettel, A. ;

Borgschulte, A. .

PHYSICAL REVIEW B, 2009, 80 (10)

← 1 2 3 4 →