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

被引:26
作者
Celik, Gokhan [1 ]
Ailawar, Saurabh A. [1 ]
Gunduz, Seval [1 ]
Miller, Jeffrey T. [2 ]
Edmiston, Paul L. [3 ]
Ozkan, Umit S. [1 ]
机构
[1] Ohio State Univ, William G Lowrie Dept Chem & Biomol Engn, 151 W Woodruff Ave, Columbus, OH 43210 USA
[2] Purdue Univ, Davidson Sch Chem Engn, 480 Stadium Mall Dr, W Lafayette, IN 47907 USA
[3] Coll Wooster, Dept Chem, 943 Coll Mall, Wooster, OH 44691 USA
基金
美国国家科学基金会;
关键词
Swellable organically-modified silica (SOMS); Palladium; Swelling; Pd/Al2O3; Hydrodechlorination; Deactivation; Hydrophobicity; SUPPORTED PALLADIUM CATALYSTS; CHLORINATED-HYDROCARBON CONTAMINANTS; BIMETALLIC NANOPARTICLE CATALYSTS; RAY-ABSORPTION SPECTROSCOPY; NOBLE-METAL CATALYSTS; PARTICLE-SIZE; SURFACE-AREA; PHOTOELECTRON-SPECTROSCOPY; CARBON NANOFIBRES; GAMMA-ALUMINA;
D O I
10.1016/j.apcatb.2018.08.065
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
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 N-2 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.
引用
收藏
页码:654 / 664
页数:11
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