Catalytic nitrate reduction in drinking water using a trickle bed reactor
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Palladium-based bimetallic catalysts hold promise as an alternative water treatment technology for nitrate (NO3-), but practical application requires development of a flow-through reactor that efficiently delivers hydrogen (H2) from the gas phase into water, where it serves as the electron donor for NO3- reduction. In this work, a trickle bed reactor (TBR) was fabricated and evaluated to address this challenge. A series of batch experiments with Pd-In/γ-Al2O3 catalysts were conducted in excess H2 to identify a highly active catalyst for the TBR. A 0.1wt%Pd-0.01wt%In on 1 mm γ-Al2O3 catalyst was selected due to its high activity and support size that promotes a uniform liquid distribution in a packed bed. The TBR was packed with the same catalyst, and various liquid and gas flow rates were tested to evaluate apparent catalyst activity. Influent and effluent NO3- concentrations were used to calculate apparent zero-order rate constants, and they generally increased with H2 flow rate. Above 900 mL/min, a change in flow regime from pulse to bubble flow was observed, and the calculated zero-order rate constants decreased. An optimal catalyst activity in the TBR of 19.5 mg NO3-/min∙g Pd was obtained at a liquid flow rate of 900 mL/min and H2 flow rate of 320 sccm, which is ~22% of the activity obtained in the batch reactor by the same catalyst, indicating H2 mass transfer limitations. A reactive transport model was developed and used to quantify H2 mass transfer rate coefficients from the liquid to gas phase. Mass transfer coefficients initially decrease and then stabilize as the H2 flow rate increases. At elevated H2 flow rates, the highest mass transfer coefficients were obtained at the 900 mL/min liquid flow rate, in agreement with activity trends. Evaluation of a larger range of liquid and gas flow rates is warranted to determine if H2 mass transfer in the TBR can be further enhanced.