Study of the hydrogenation mechanism of LaCuMg8 ternary phase: The decomposition induces kinetics improvement

被引:25
作者
Couillaud, S. [1 ]
Gaudin, E. [1 ]
Andrieux, J. [2 ]
Gorsse, S. [1 ]
Gayot, M. [1 ]
Bobet, J. L. [1 ]
机构
[1] Univ Bordeaux, CNRS, ICMCB, F-33600 Pessac, France
[2] European Synchrotron Radiat Facil, F-33043 Grenoble, France
关键词
Rare-earth intermetallics; Hydrogen storage; Kinetic and thermodynamic study; Morphologic effects; STORAGE PROPERTIES; MAGNESIUM; SORPTION; LA2MG17; ALLOYS; MG; HYDRIDES; GD;
D O I
10.1016/j.ijhydene.2012.05.025
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 sorption properties of LaCuMg8 are investigated. LaCuMg8 crystallizes in the La2Mg17 structure type with the lattice parameters a = 10.1254(2) angstrom and c = 10.0751(2) angstrom. An absorption mechanism in 2 steps was reported earlier: (i) the first step, which is irreversible, induces the decomposition of LaCuMg8 into an intimate mixture of 3 phases of sub-micronic size (i.e. LaH3, MgCu2 and MgH2); (ii) the second step consists in the reversible absorption of the "LaCuMg8 activated powder" with kinetics better than for pure magnesium. In order to get a better understanding of the absorption process, it was investigated from thermodynamic, kinetic and morphology points of view. From thermodynamic point of view, the "LaCuMg8 activated powder" behaves like a mixture. Concerning the kinetics, the activation energy was evaluated at about 65 kJ/mol H-2, using Avrami-Erofeev model and Arrhenius law. To explain the enhancement of the kinetics, both effects of (i) Mg2Cu/MgCu2 transformation and (ii) morphology induced by the decomposition have been considered. Copyright (C) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:11824 / 11834
页数:11
相关论文
共 37 条
[21]   Electrochemical properties of AB5-type hydride-forming compounds prepared by mechanical alloying [J].
Lenain, C ;
Aymard, L ;
Salver-Disma, F ;
Leriche, JB ;
Chabre, Y ;
Tarascon, JM .
SOLID STATE IONICS, 1997, 104 (3-4) :237-248
[22]   Catalytic effect of transition metals on hydrogen sorption in nanocrystalline ball milled MgH2-Tm (Tm=Ti, V, Mn, Fe and Ni) systems [J].
Liang, G ;
Huot, J ;
Boily, S ;
Van Neste, A ;
Schulz, R .
JOURNAL OF ALLOYS AND COMPOUNDS, 1999, 292 (1-2) :247-252
[23]   Thermodynamic and ab initio investigation of the A1-H-Mg system [J].
Palumbo, A. ;
Torres, F. J. ;
Ares, J. R. ;
Pisani, C. ;
Fernandez, J. F. ;
Baricco, A. .
CALPHAD-COMPUTER COUPLING OF PHASE DIAGRAMS AND THERMOCHEMISTRY, 2007, 31 (04) :457-467
[24]   REACTION OF HYDROGEN WITH ALLOYS OF MAGNESIUM AND COPPER [J].
REILLY, JJ ;
WISWALL, RH .
INORGANIC CHEMISTRY, 1967, 6 (12) :2220-&
[25]   REACTION HYDROGEN WITH ALLOYS MAGNESIUM AND NICKEL AND FORMATION OF MG2NIH4 [J].
REILLY, JJ ;
WISWALL, RH .
INORGANIC CHEMISTRY, 1968, 7 (11) :2254-&
[26]   The application of Mg-based metal-hydrides as heat energy storage systems [J].
Reiser, A ;
Bogdanovic, B ;
Schlichte, K .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2000, 25 (05) :425-430
[27]   RECENT ADVANCES IN MAGNETIC-STRUCTURE DETERMINATION BY NEUTRON POWDER DIFFRACTION [J].
RODRIGUEZCARVAJAL, J .
PHYSICA B, 1993, 192 (1-2) :55-69
[28]  
Schulz R, 1999, Patent, Patent No. [09/424,331, 09424331]
[29]   MAGNESIUM AND MAGNESIUM ALLOY HYDRIDES [J].
SELVAM, P ;
VISWANATHAN, B ;
SWAMY, CS ;
SRINIVASAN, V .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 1986, 11 (03) :169-192
[30]   Preparation and hydrogen storage properties of nanostructured Mg2Cu alloy [J].
Shao, HY ;
Wang, YT ;
Xu, HR ;
Li, XG .
JOURNAL OF SOLID STATE CHEMISTRY, 2005, 178 (07) :2211-2217