Hydration of γ-alumina in water and its effects on surface reactivity

被引:221
作者
Lefèvre, G
Duc, M
Lepeut, P
Caplain, R
Fédoroff, M
机构
[1] Ctr Etud Chim Met, CNRS UPR2801, F-94407 Vitry Sur Seine, France
[2] Conservatoire Natl Arts & Metiers, Lab Ceram, Chaire Mat Ind Met & Ceram, F-75141 Paris 03, France
关键词
D O I
10.1021/la025651i
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The stability of y-alumina suspensions in water has been investigated by long-duration experiments (1 day to 6 months). Several complementary methods were used to characterize the solid (acid-base titration and dissolution rate measurements, X-ray photoelectron spectroscopy, X-ray diffraction, gravimetric/differential thermal analysis, infrared spectroscopy, and scanning electron microscopy). It appears that y-alumina, which is widely used as a model oxide in sorption experiments, thanks mainly to its high specific surface area and to the presence of aluminol groups on its surface, is progressively transformed to bayerite (beta-Al(OH)(3)).' This transformation was characterized by an induction period of about 4 days, corresponding to the formation, of a transient amorphous hydrated phase, followed by an increase in the bayerite concentration, which levels off after about 2 months. This transformation results in a dramatic decrease in the surface density of sites reactive to protons. Thermodynamical calculations predict the hydration reaction of y-alumina leading to a more stable phase (bayerite, gibbsite, or boebmite). Since the surface reactivity and sorption properties of solids are factors controlling the transport of elements in water, it is necessary to take into account the stability of solids when modeling sorption experiments. These factors are important for the long-term prediction of the effectiveness of barriers placed around radioactive waste depositories.
引用
收藏
页码:7530 / 7537
页数:8
相关论文
共 34 条
[1]  
[Anonymous], 1976, OXIDES OXIDE FILMS
[2]   INVESTIGATION OF THE THERMODYNAMIC PROPERTIES OF GAMMA-AL2O3 [J].
CHEN, QY ;
ZENG, WM ;
CHEN, XM ;
GU, SQ ;
YANG, GQ ;
ZHOU, HF ;
YIN, ZL .
THERMOCHIMICA ACTA, 1995, 253 :33-39
[3]  
DAVIS JA, 1990, REV MINERAL, V23, P177
[4]  
DEBONTRIDDER F, 2001, THESIS U PARIS 11 PA
[5]   SURFACE HYDRATION OF AQUEOUS GAMMA-AL2O3 STUDIED BY FOURIER-TRANSFORM RAMAN AND INFRARED-SPECTROSCOPY .1. INITIAL RESULTS [J].
DYER, C ;
HENDRA, PJ ;
FORSLING, W ;
RANHEIMER, M .
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 1993, 49 (5-6) :691-705
[6]   THE COORDINATION CHEMISTRY OF WEATHERING .1. DISSOLUTION KINETICS OF DELTA-AL2O3 AND BEO [J].
FURRER, G ;
STUMM, W .
GEOCHIMICA ET COSMOCHIMICA ACTA, 1986, 50 (09) :1847-1860
[7]   MULTISITE PROTON ADSORPTION MODELING AT THE SOLID-SOLUTION INTERFACE OF (HYDR)OXIDES - A NEW APPROACH .1. MODEL DESCRIPTION AND EVALUATION OF INTRINSIC REACTION CONSTANTS [J].
HIEMSTRA, T ;
VANRIEMSDIJK, WH ;
BOLT, GH .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 1989, 133 (01) :91-104
[8]  
Hiemstra T, 1999, LANGMUIR, V15, P5942
[9]   MULTISITE PROTON ADSORPTION MODELING AT THE SOLID-SOLUTION INTERFACE OF (HYDR)OXIDES - A NEW APPROACH .2. APPLICATION TO VARIOUS IMPORTANT (HYDR)OXIDES [J].
HIEMSTRA, T ;
DEWIT, JCM ;
VANRIEMSDIJK, WH .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 1989, 133 (01) :105-117
[10]   INTERACTION OF PB-2+ WITH HYDROUS GAMMA-AL-2O-3 [J].
HOHL, H ;
STUMM, W .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 1976, 55 (02) :281-288