Studying the basic characteristics and photocatalytic properties of graphitic carbon nitride prepared from the desulfurized waste liquid secondary salt component

Abstract

The desulfurized waste liquid (DWL) produced in the process of wet oxidation removal of hydrogen sulfide (H2S) and hydrogen cyanide (HCN) from coke oven gas is rich in ammonium thiocyanate (NH4SCN), ammonium thiosulfate ((NH4)2S2O3), and ammonium sulfate ((NH)2SO4). Based on the research of thermal decomposition of DWL, the study on the preparation of graphitic carbon nitride (g-C3N4) by thermal polymerization in hydrogen (H2) atmosphere using the salts of DWL as precursor was carried out. Specifically, a single salt (NH4SCN), a double salt combination (NH4SCN + (NH)2SO4) or (NH4SCN + (NH4)2S2O3), and a three salt combination (NH4SCN + (NH)2SO4 + (NH4)2S2O3) were used as precursors to prepare g-C3N4. The morphology, phase composition, specific surface area, pore structure distribution, element composition, element valence distribution, and light absorption characteristics of the prepared samples were characterized. The performance of the prepared samples was evaluated by photocatalytic degradation of rhodamine B under visible light. The characterization results showed that the product (CN-MIX) obtained by the pyrolysis of three salt combination has a most fluffy and porous structure with the maximum specific surface area of 56.89 m2/g. Which can be attributed to the template effect of the gases produced by the pyrolysis of (NH4)2S2O3 and (NH)2SO4 accompanying the deamination and polycondensation of the intermediate product from the pyrolysis of NH4SCN. CN-MIX has a widest band gap of 2.93eV with a more negative conduction band. After 4 h of visible light irradiation, the degradation rates of 300 mL rhodamine B solution (60 mg/L) photocatalyzed by 50 mg mono-salt product and tri-salt product catalyst were 58.27% and 96.49% respectively. This is due to the synergistic effect of the large specific surface area, abundant structural defects and the strong reduction ability of photo-generated electrons in CN-MIX. The great photocatalytic performance of CN-MIX has positive theoretical guiding significance for the preparation of highly active photocatalyst g-C3N4 by using the mixed salt of desulfurized waste liquid.