Highly selective chemical reduction of nitrate in water in carbon-based contactor catalytic membrane reactors

Abstract

A carbon-based catalytic membrane reactor in a contactor (interfacial) configuration has been used as an approach to control selectivity in the reduction of NO3- in water. Water and hydrogen fed to the reactor circulate tangentially on opposite sides of the membrane, which acts as a separator and contactor, enabling hydrogen transfer to the water phase. Powdered carbons (carbon black, carbon nanofiber, and activated carbon) were used to prepare catalytic membranes that also acted as contactors to transfer H2 from the gas phase to water. The membranes based on the Pd-Cu/carbon black catalyst showed lower selectivity towards unwanted NH4+ than the Pd-Cu and Pd-Sn catalysts supported on carbon nanofibers and activated carbon, due to a good balance among conductivity, external surface area, and particle size. Sensitivity analysis for H2 partial pressure demonstrated that the contactor membrane reactor can be operated with control of H2 mass transfer, hence enabling enhanced control of the selectivity to NH4+. Additional control of selectivity was achieved by reducing the catalytic layer thickness of the membrane, which improved NO3- transport and decreased the H/N ratio at the active centers. With these approaches, NO3- conversion values above 40 % with negligible NH4+ production and NO3- conversions close to 60 % with NH4+ selectivity values around 3 % were achieved.