Aqueous-phase hydrodechlorination of trichloroethylene over Pd-based swellable organically-modified silica (SOMS): Catalyst deactivation due to chloride anions

[Display omitted] •Swellable Organically-Modified Silica (SOMS) was used as a catalyst scaffold.•The resistance of Pd/SOMS and Pd/Al2O3 against chloride anions was examined.•Formation of Pd-Cl complexes and loss of catalytic activity were observed over Pd/Al2O3.•The accelerated poisoning experiments...

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Veröffentlicht in:Applied catalysis. B, Environmental Environmental, 2018-12, Vol.239 (C), p.654-664
Hauptverfasser: Celik, Gokhan, Ailawar, Saurabh A., Gunduz, Seval, Miller, Jeffrey T., Edmiston, Paul L., Ozkan, Umit S.
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Sprache:eng
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Zusammenfassung:[Display omitted] •Swellable Organically-Modified Silica (SOMS) was used as a catalyst scaffold.•The resistance of Pd/SOMS and Pd/Al2O3 against chloride anions was examined.•Formation of Pd-Cl complexes and loss of catalytic activity were observed over Pd/Al2O3.•The accelerated poisoning experiments did not affect the textural properties of Pd/SOMS.•Pd/SOMS showed excellent resistance to chloride poisoning and metal leaching. Swellable-organically modified silica (SOMS) has been demonstrated to be an efficient catalyst scaffold for catalytic treatment of water contaminated with trichloroethylene (TCE). In this study, deactivation characteristics of Pd-incorporated SOMS for aqueous-phase hydrodechlorination (HDC) of TCE were investigated. Pd/SOMS catalysts were exposed to highly-concentrated chloride solutions (up to 1 M NaCl or 0.01 M HCl) to examine the deactivation resistant behavior of Pd/SOMS. The commonly used HDC catalyst Pd/Al2O3 was also studied for comparison purposes. Pd/SOMS and Pd/Al2O3 in their pristine and treated states were tested for aqueous-phase HDC of TCE and characterized by several techniques including N2 physisorption, inductively coupled plasma optical emission spectroscopy (ICP-OES), X-ray photoelectron spectroscopy, extended X-ray absorption fine structure spectroscopy (EXAFS), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) of adsorbed CO. The aqueous-phase treatments had a pronounced adverse effect on the textural properties of Pd/Al2O3, although the effect was independent of the type of the chloride precursor, NaCl or HCl. Treating Pd/Al2O3 with chloride-containing solutions lowered the catalytic activity due to formation of Pd-Cl complexes and active metal leaching. The leached Pd obtained from the treatment solution was shown to be inactive for aqueous-phase HDC of TCE. While Pd/Al2O3 underwent severe deactivation due to the chloride treatments, Pd/SOMS exhibited resistance to chloride deactivation and metal leaching. The chloride treatments did not impact the textural properties of Pd/SOMS. The achieved deactivation resistance was attributed to the novel characteristics of the SOMS support.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2018.08.065