Exhaustive Conversion of Inorganic Nitrogen to Nitrogen Gas Based on a Photoelectro-Chlorine Cycle Reaction and a Highly Selective Nitrogen Gas Generation Cathode

Abstract

A novel method for the exhaustive conversion of inorganic nitrogen to nitrogen gas is proposed in this paper. The key properties of the system design included an exhaustive photoelectrochemical cycle reaction in the presence of Cl^-, in which Cl· generated from oxidation of Cl^- by photoholes selectively converted NH₄⁺ to nitrogen gas and some NO₃^- or NO₂^-. The NO₃^- or NO₂^- was finally reduced to nitrogen gas on a highly selective Pd-Cu-modified Ni foam (Pd-Cu/NF) cathode to achieve exhaustive conversion of inorganic nitrogen to nitrogen gas. The results indicated total nitrogen removal efficiencies of 30 mg L^-1 inorganic nitrogen (NO₃^-, NH₄⁺, NO₃^-/NH₄⁺ = 1:1 and NO₂^-/NO₃^-/NH₄⁺ = 1:1:1) in 90 min were 98.2%, 97.4%, 93.1%, and 98.4%, respectively, and the remaining nitrogen was completely removed by prolonging the reaction time. The rapid reduction of nitrate was ascribed to the capacitor characteristics of Pd-Cu/NF that promoted nitrate adsorption in the presence of an electric double layer, eliminating repulsion between the cathode and the anion. Nitrate was effectively removed with a rate constant of 0.050 min^-1, which was 33 times larger than that of Pt cathode. This system shows great potential for inorganic nitrogen treatment due to the high rate, low cost, and clean energy source.