Activity and stability of the catalytic hydrogel membrane reactor for treating oxidized contaminants

The catalytic hydrogel membrane reactor (CHMR) is an interfacial membrane process that uses nano-sized catalysts for the hydrogenation of oxidized contaminants in drinking water. In this study, the CHMR was operated as a continuous-flow reactor using nitrite (NO₂^-) as a model contaminant and palladium (Pd) as a model catalyst. Using the overall bulk reaction rate for NO₂^- reduction as a metric for catalytic activity, we evaluated the effect of the hydrogen gas (H₂) delivery method to the CHMR, the initial H₂ and NO₂^- concentrations, Pd density in the hydrogel, and the presence of Pd-deactivating species. The chemical stability of the catalytic hydrogel was evaluated in the presence of aqueous cations (H⁺, Na⁺, Ca²⁺) and a mixture of ions in a hard groundwater. Delivering H₂ to the CHMR lumens using a vented operation mode, where the reactor is sealed and the lumens are periodically flushed to the atmosphere, allowed for a combination of a high H₂ consumption efficiency and catalytic activity. The overall reaction rate of NO₂^- was dependent on relative concentrations of H₂ and NO₂^- at catalytic sites, which was governed by both the chemical reaction and mass transport rates. The intrinsic catalytic reaction rate was combined with a counter-diffusional mass transport component in a 1-D computational model to describe the CHMR. Common Pd-deactivating species [sulfite, bisulfide, natural organic matter] hindered the reaction rate, but the hydrogel afforded some protection from deactivation compared to a batch suspension. No chemical degradation of the hydrogel structure was observed for a model water (pH > 4, Na⁺, Ca²⁺) and a hard groundwater after 21 days of exposure, attesting to its stability under natural water conditions.