期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 291, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120060
关键词
Pd supported on swellable organically modified; silica (SOMS); Hydrodechlorination; Catalyst deactivation; Trichloroethylene; In-situ X-ray absorption near edge spectroscopy; (XANES); Hydrophobicity
资金
- National Science Foundation [CBET-1436729]
- Ohio Coal Research Consortium
- National Science Foundation Energy Research Center for Innovative and Strategic Transformation of Alkane Resources (CISTAR) [EEC1647722]
- Department of Energy
- MRCAT member institutions
- DOE Office of Science [DEAC0206CH11357]
This study investigates the dual role of trichloroethylene (TCE) in liquid-phase hydrodechlorination with Pd catalysts supported on swellable organically modified silica (SOMS). The results show that TCE acts as both a reactant and a swelling-agent, with economic viability for the hydrodechlorination process.
Herein, the dual role of trichloroethylene (TCE) in liquid-phase hydrodechlorination with Pd catalysts supported on swellable organically modified silica (SOMS), is investigated. Batch experiments with TCE-soaked Pd/SOMS showed 45% higher conversion after 4 h than dry Pd/SOMS, suggesting that TCE acts as a reactant and as a swelling-agent. Flow experiments performed with and without ethanol (external swelling-agent) exhibited similar steady-state activities, confirming that TCE itself can cause swelling. Moreover, flow experiments, regardless of whether the SOMS-supported Pd catalysts were pre-reduced or not, yielded similar steady-state conversions, suggesting that Pd(2+) is rapidly reduced by H2 dissolved in water during approach to steadystate. In-situ characterization performed under reaction conditions using time-resolved X-ray absorption spectroscopy confirmed the reduction of Pd(2+) species to Pd(0) by dissolved H2. Overall, this study shows economic viability of hydrodechlorination of TCE using Pd/SOMS by eliminating the need for an external swelling-agent as well as a catalyst pre-reduction step.
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