4.8 Article

Long-Term Continuous Co-reduction of 1,1,1-Trichloroethane and Trichloroethene over Palladium Nanoparticles Spontaneously Deposited on H2-Transfer Membranes

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ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 55, 期 3, 页码 2057-2066

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AMER CHEMICAL SOC
DOI: 10.1021/acs.est.0c05217

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资金

  1. U.S. Department of Defense (DOD) Strategic Environmental Research and Development Program (SERDP) [ER-2721]
  2. National Science Foundation Nanosystems Engineering Research Center on Nanotechnology-Enabled Water Treatment (NEWT) [EEC-1449500]
  3. Nanotechnology Collaborative Infrastructure Southwest [NNCI-ECCS-1542160]

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The study investigated the co-reduction of 1,1,1-TCA and TCE using PdNP catalysts deposited on H-2-transfer membranes, achieving high catalytic activity and stability with effective reduction of contaminant concentrations to non-toxic ethane as the main product.
1,1,1-Trichloroethane (1,1,1-TCA) and trichloroethene (TCE) are common recalcitrant contaminants that coexist in groundwater. H-2-induced reduction over precious-metal catalysts has proven advantageous, but its application to long-term continuous treatment has been limited due to poor H-2-transfer efficiency and catalyst loss. Furthermore, catalytic reductions of aqueous 1,1,1-TCA alone or concomitant with TCE catalytic co-reductions are unstudied. Here, we investigated 1,1,1-TCA and TCE co-reduction using palladium nanoparticle (PdNP) catalysts spontaneously deposited on H-2-transfer membranes that allow efficient H-2 supply on demand in a bubble-free form. The catalytic activities for 1,1,1-TCA and TCE reductions reached 9.9 and 11 L/g-Pd/min, values significantly greater than that reported for other immobilized-PdNP systems. During 90 day continuous operation, removals were up to 95% for 1,1,1-TCA and 99% for TCE. The highest steady-state removal fluxes were 1.5 g/m(2)/day for 1,1,1-TCA and 1.7 g/m(2)/day for TCE. The major product was nontoxic ethane (94% selectivity). Only 4% of the originally deposited PdNPs were lost over 90 days of continuous operation. Documenting long-term continuous Pd-catalyzed dechlorination at high surface loading with minimal loss of the catalyst mass or activity, this work expands understanding of and provides a foundation for sustainable catalytic removal of co-existing chlorinated solvents.

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