TY - JOUR
T1 - Impact of membrane immobilization on particle formation and trichloroethylene dechlorination for bimetallic Fe/Ni nanoparticles in cellulose acetate membranes
AU - Meyer, D. E.
AU - Bhattacharyya, D.
PY - 2007/6/28
Y1 - 2007/6/28
N2 - The use of membrane immobilization to carry out the batch dechlorination of trichloroethylene (TCE) using bimetallic Fe/Ni (4:1, Fe to Ni) nanoparticles in cellulose acetate membranes is examined using modeling of transport phenomenon based on experimental results. Membranes are synthesized using both gelation and solvent evaporation techniques for phase inversion. The reduction of metal ions within cellulose acetate phase-inversion membranes was accomplished using sodium borohydride reduction to obtain up to 2 wt % total metals. Characterization of the mixed-matrix structure reveals a bimodal particle distribution ranging between 18 and 80 nm within the membrane cross section. The distribution is the result of changes in the morphology of the cellulose acetate support. The diffusivity and linear partitioning coefficient for the chlorinated organic were measured and are 2.0 × 10-8 cm 2.s-1 and 3.5 × 10-2 L.g-1, respectively. An unsteady-state model for diffusion through a membrane with reaction was developed to predict experimental results with an error of only 7.2%. The error can be attributed to the lack of the model to account for loss of reactivity through pH effects, alloy effects (bimetallic ratio), and oxidation of nanoparticles. Simulations were run to vary the major transport variables, partitioning and diffusivity, and determine their impact on reaction kinetics. Of the two, diffusivity was less significant because it really only influences the time required for maximum TCE partitioning to the membrane to be achieved and has no effect on the limiting capacity of the membrane for TCE. Therefore, selection of an appropriate support material is crucial for development of highly reactive mixed-matrix membrane systems.
AB - The use of membrane immobilization to carry out the batch dechlorination of trichloroethylene (TCE) using bimetallic Fe/Ni (4:1, Fe to Ni) nanoparticles in cellulose acetate membranes is examined using modeling of transport phenomenon based on experimental results. Membranes are synthesized using both gelation and solvent evaporation techniques for phase inversion. The reduction of metal ions within cellulose acetate phase-inversion membranes was accomplished using sodium borohydride reduction to obtain up to 2 wt % total metals. Characterization of the mixed-matrix structure reveals a bimodal particle distribution ranging between 18 and 80 nm within the membrane cross section. The distribution is the result of changes in the morphology of the cellulose acetate support. The diffusivity and linear partitioning coefficient for the chlorinated organic were measured and are 2.0 × 10-8 cm 2.s-1 and 3.5 × 10-2 L.g-1, respectively. An unsteady-state model for diffusion through a membrane with reaction was developed to predict experimental results with an error of only 7.2%. The error can be attributed to the lack of the model to account for loss of reactivity through pH effects, alloy effects (bimetallic ratio), and oxidation of nanoparticles. Simulations were run to vary the major transport variables, partitioning and diffusivity, and determine their impact on reaction kinetics. Of the two, diffusivity was less significant because it really only influences the time required for maximum TCE partitioning to the membrane to be achieved and has no effect on the limiting capacity of the membrane for TCE. Therefore, selection of an appropriate support material is crucial for development of highly reactive mixed-matrix membrane systems.
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U2 - 10.1021/jp070972u
DO - 10.1021/jp070972u
M3 - Article
C2 - 17530798
AN - SCOPUS:34447511497
SN - 1520-6106
VL - 111
SP - 7142
EP - 7154
JO - Journal of Physical Chemistry B
JF - Journal of Physical Chemistry B
IS - 25
ER -