Long-Term Continuous Co-reduction of 1,1,1-Trichloroethane and Trichloroethene over Palladium Nanoparticles Spontaneously Deposited on H_2-Transfer Membranes

摘要

1,1,1-TrichIoroethane (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~2Vday 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.