Homogeneous Ni(I)tetra Sulfonated Phthalocyanine Electrocatalyst Generated at Low Overpotential Clubbed with a Wet-Scrubbing Column for High Efficiency NO Reduction to NH3

摘要

Although the degradation of NO gas to a less toxic form is a promising strategy to help solve atmospheric health and ozone depletion problems, conversion to a useful gas is a recent strategy. The generation of NH3 from NO with high efficiency per catalyst area or weight is in the early stages. In this investigation, a tetra sulfonated phthalocyanine with a Ni(II) (Ni(II)TSPc) complex was used to produce a low valent homogenous electrocatalyst Ni(I)TSPc in an alkaline medium at a lower overpotential. Ni(I)TSPc formation at a lower overpotential was demonstrated by the initial change in oxidation/reduction potential from 25 mV to -360 mV during electrolysis, peak potential change in cyclic voltammetry, and UV-Vis spectral analysis. A potentiometric titration method used to quantify the electrogenerated Ni(I)TSPc revealed 90 % efficiency in 1 h. The decrease of Ni(I)TSPc concentration when contacting NO gas at the wet scrubber column showed that the NO removal process followed a Ni(I)TSPc (Ni(I)) mediation or mediated electrocatalytic reduction (MER) process. The NO removal efficiency reached almost 100 % at a 0.2 L/min gas flow rate of 20 ppm. The selective formation of NH3 with a maximum of 1492 mu mol/g Ni(I) was achieved for the first time in the homogeneous electrocatalytic reduction process. The developed process generated NH3 from NO gas and has the potential for scale-up.