Superior reduction of nitrate with simultaneous oxidation of intermediates and enhanced nitrogen gas selectivity via novel electrochemical treatment

Abstract

This study reports an electrochemical reduction of the NO3− along with oxidation of the in-situ generated NH4+ with maximum selectivity of the N2 gas as the final-product. The use of aluminum as a cathode and Ti/RuO2 as an anode showed enhanced electrochemical nitrate reduction at the cathode and oxidation of the ammonium ion at the anode. Effects of various parameters like initial NO3− concentration (Co = 100−400 mg L−1), a dose of the Cl− as NaCl (NaCl = 100−400 mg L−1), current density applied (j = 83.3-333.3 A m−2), solution pH (pH = 4–10) and electrolysis time (t = 0−120 min) were studied in terms of NO3− reduction and total nitrogen (TN) removal efficiencies. Current efficiency (CE) was elaborated with respect to end products like N2, NO2− and NH4+. Specific electrical energy consumption (SEC) was calculated in kWh kg−1 NO3− removed for the electrochemical process. Electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) were utilized for understanding the oxidation/reduction mechanism over electrodes and the characteristics of the electrodes in a different solution. The studied mechanism suggested a circular conversion of NO3− through complex processes into the N2 gas as the final product. The ultimate nitrate and TN degradation efficiency of ≈95 % with N2 selectivity of ≈100 % were achieved at the optimum condition of Co = 100 mg L−1, NaCl = 300 mg L−1, j = 333.3 A m−2, pH = 6 and time = 120 min with SEC = 927.4 kW h kg−1 NO3− removed. The 1st, 2nd, and nth-order kinetic models were used for the reaction kinetics. FE-SEM, XRD, and AFM techniques were used for the characterization of the electrodes before and after all the electrochemical runs. The operating cost was calculated for lab-scale treatment along with a comparison with previous studies. No sludge or scum got produced for each electrochemical run. Finally, this study delivers a superior perceptive for electrochemical characteristics of Al at the cathode side and Ti/RuO2 at anode side as well as electrochemical NO3− reduction and oxidation of the generated NH4+, simultaneously.