Optimization of nitrogen-doped sludge char preparation and mechanism study for catalytic oxidation of NO at room temperature

Abstract

Catalytic oxidation of NO at room temperature was carried out over nitrogen (N)-doped sludge char (SC) prepared from pyrolysis of municipal sewage sludge, and urea was adopted as nitrogen source. The effects of different N-doping methods (one-step and two-step method), dried sludge (DS)/urea mass ratios (5:1, 4:1, 3:1, 2:1, and 1:1), SC preparation procedures (pyrolysis only, pyrolysis with acid washing, and pyrolysis with KOH activation and acid washing), and different pyrolysis temperatures (500, 600, 700, and 800°C) on the catalytic oxidation of NO were compared to optimize the procedure for SC preparation. The results indicated that N-doping could obviously promote the catalytic performance of SC. The one-step method with simultaneous sludge pyrolysis (at 700°C), KOH activation, and N-doping (DS/urea of 3:1) was the optimal procedure for preparing the N-doped SC with the NO conversion rate of 54.7%, whereas the optimal NO conversion rate of SC without N-doping was only 47.3%. Urea worked both as carbon and nitrogen source, which could increase about 2.9%-16.5% of carbon and 24.8%-42.7% of nitrogen content in SC pyrolyzed at 700°C. N-doping significantly promoted microporosity of SC. The optimal N-doped SC showed specific surface areas of 571.38 m2/g, much higher than 374.34 m2/g of the optimal SC without N-doping. In addition, N-doping also increased amorphousness and surface basicity of SC through the formation of N-containing groups. Finally, three reaction paths, i.e. microporous reactor, active sites, and basic site control path, were proposed to explain the mechanism of N-doping on promoting the catalytic performance of NO.