Electrochemical reduction of nitrate in a catalytic carbon membrane nano-reactor

Abstract

Nitrate pollution is a critical environmental issue in need of urgent addressing. Electrochemical reduction is an attractive strategy for treating nitrate due to the environmental friendliness. However, it is still a challenge to achieve the simultaneous high activity and selectivity. Here we report the design of a porous tubular carbon membrane as the electrode deposited with catalysts, which provides a large triple-phase boundary area for nitrate removal reactions. The achieved nitrate removal rate is one order of magnitude higher than other literatures with high nitrate conversion and high selectivity of nitrogen. The carbon membrane itself had a limited catalytic property thus Cu-Pd bimetal catalysts were deposited inside the nano-pores to enhance the activity and selectivity. When Na2SO4 electrolyte was applied, the achieved single-pass removal of nitrate was increased from 55.15% (for blank membrane) to 97.12% by adding catalysts inside the membrane. In case of NaOH as the electrolyte, the single-pass nitrate removal efficiency, selectivity to nitrogen formation and nitrate removal rate was 90.66%, 96.40% and 1.47 × 10−3 mmol min−1 cm−2, respectively. Density functional theory studies demonstrate that the loading of bimetal catalysts compared with single metal catalysts enhances the adsorption of *NO3 on membrane surface favorable for N2 formation than NH3 on Cu-Pd surface. The application of catalytic carbon membrane nano-reactors can open new windows for nitrate removal due to the high reactor efficiency.