The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, School of Environment and Energy, South China University of Technology, Guangzhou, 510006, PR China. Electronic address: [Email]
The development of a new class of carbon electrocatalysts for nitrate reduction reaction (NRR) that have high activity and durability is extremely important, as currently reported metallic electrocatalysts show a main drawback of low stability owing to leaching and oxidation. Herein, we demonstrate that a unique N-doped graphitic carbon-encapsulated iron nanoparticles can be utilized as a promising NRR electrocatalyst. The resulting Fe(20%)@N-C achieves a better nitrate removal proportion of 83.0% (attained in the first running cycle) compared to the efficiencies of other reference catalysts, including those with lower entrapped Fe content. The nitrogen selectivity is 25.0% in the absence of Cl- and increases to 100% when supplemented with 1.0 g L-1 NaCl. More importantly, there is no statistically significant difference (at a 95% confidence interval) regarding the removal percentage recorded over 20 cycles for the Fe(20%)@N-C cathode. We propose that the iron nanoparticles could attenuate the work function on the neighboring carbon atoms, which are the reactive sites for NRR, and that the graphitic shells hinder the access of the electrolyte, thus protecting the iron particles from dissolution and oxidation. Testing with the real industrial wastewater further demonstrates the superiority of Fe(20%)@N-C cathode towards NRR, as evidenced by efficient removal of nitrate available in the biological effluent from a local coking wastewater treatment plant.