Effects of surface activity, defects and mass transfer on hydrogen permeance and n-value in composite palladium-porous stainless steel membranes

被引:98
作者
Guazzone, Federico [1 ]
Engwall, Erik Edwin [1 ]
Ma, Yi Hua [1 ]
机构
[1] Worcester Polytech Inst, Dept Chem Engn, Ctr Inorgan Membrane Studies, Worcester, MA 01609 USA
关键词
n-value; hydrogen penneance; hydrogen flux; palladium membranes; surface poisoning; leaks; selectivity;
D O I
10.1016/j.cattod.2005.12.010
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The H-2 permeance of composite palladium-porous stainless steel (Pd-PSS) membranes was determined: (1) by assuming Sieverts' law (n = 0.5) and (2) by performing a non-linear fit in order to obtain the hydrogen permeance and the n-value. For all membranes (thickness > 15 mu m) the n-value was higher than 0.6 at low temperatures (< 350 degrees C) and close to 0.5 at higher temperatures (> 400 degrees C). The activation of the membrane with the surface either seeded withpalladium or oxidized in air at 350 degrees C for 48 h led to lower n-values indicating that the surface reaction rate even in thick membranes with selectivities (H-2/He) above 400 might still contribute, though to a minor extent, to the overall hydrogen permeation mechanism. For leaky membranes (selectivity << 400) the Knudsen diffusion and viscous flow of molecular H2 through the defects led to n-values as high as 0.75 at 500 degrees C. n-Values higher than 0.5 were also found for Pd-PSS membranes when the PSS support had a large resistance. (c) 2006 Elsevier B.V. All rights reserved.
引用
收藏
页码:24 / 31
页数:8
相关论文
共 29 条
[1]   Spontaneous ordering of oxide nanostructures [J].
Aggarwal, S ;
Monga, AP ;
Perusse, SR ;
Ramesh, R ;
Ballarotto, V ;
Williams, ED ;
Chalamala, BR ;
Wei, Y ;
Reuss, RH .
SCIENCE, 2000, 287 (5461) :2235-2237
[2]   DEACTIVATION AND REGENERATION OF PD-AG MEMBRANES FOR DEHYDROGENATION REACTIONS [J].
ALI, JK ;
NEWSON, EJ ;
RIPPIN, DWT .
JOURNAL OF MEMBRANE SCIENCE, 1994, 89 (1-2) :171-184
[3]   METAL COMPOSITE MEMBRANES FOR HYDROGEN SEPARATION [J].
ATHAYDE, AL ;
BAKER, RW ;
NGUYEN, P .
JOURNAL OF MEMBRANE SCIENCE, 1994, 94 :299-311
[4]   Nanostructured palladium-iron membranes for hydrogen separation and membrane hydrogenation reactions [J].
Bryden, KJ ;
Ying, JY .
JOURNAL OF MEMBRANE SCIENCE, 2002, 203 (1-2) :29-42
[5]   PREPARATION AND CHARACTERIZATION OF A COMPOSITE PALLADIUM-CERAMIC MEMBRANE [J].
COLLINS, JP ;
WAY, JD .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1993, 32 (12) :3006-3013
[6]   Methane conversion to syngas in a palladium membrane reactor [J].
Galuszka, J ;
Pandey, RN ;
Ahmed, S .
CATALYSIS TODAY, 1998, 46 (2-3) :83-89
[7]   Increase of Pd surface area by treatment in dioxygen [J].
Han, JY ;
Zhu, GH ;
Zemlyanov, DY ;
Ribeiro, FH .
JOURNAL OF CATALYSIS, 2004, 225 (01) :7-15
[8]   DIFFUSION OF HYDROGEN THROUGH PALLADIUM [J].
HURLBERT, RC ;
KONECNY, JO .
JOURNAL OF CHEMICAL PHYSICS, 1961, 34 (02) :655-&
[9]   Efficient hydrogen production via methanol steam reforming by preventing back-permeation of hydrogen in a palladium membrane reactor [J].
Itoh, N ;
Kaneko, Y ;
Igarashi, A .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2002, 41 (19) :4702-4706
[10]  
JAYARAMAN V, 1995, J MEMBRANE SCI, V104, P241