Sulfate radical-advanced oxidation process (SR-AOP) for simultaneous removal of refractory organic contaminants and ammonia in landfill leachate

摘要

Typically, a mature landfill leachate contains high levels of non-biodegradable organics and ammonia nitrogen. Simultaneous removal of the both persistent leachate pollutants is a significant challenge. This paper reports the first scientific study to apply a sulfate radical (SO_4~-) — based advanced oxidation process (SR-AOP) to treat a mature leachate, with an emphasis of concurrent removal of refractory organics and ammonia. In this study, all the experiments were run in a batch reactor with temperature control. In the thermal per-sulfate oxidation (TPO) process, persulfate (S_2O_8~(2-)) was activated by heat to produce powerful oxidants, SO_4~- (E° = 2.6 V). Three factors affecting the removal efficiencies of chemical oxygen demand (COD) and ammonia nitrogen were investigated, including initial solution pH (3-8.3), temperature (27-50 ℃), and chemical dose (S_2O_8~(2-) :12COD_0 = 0.25-2.0). Typically, acidic pH (3—4), higher temperature, and higher dose favored the removal of COD and ammonia. At S_2O_8~(2-):12COD_0 = 2 and 50 ℃, the COD removal rates were 79% and 91% at pH 8.3 (no pH adjustment) and 4, respectively; and the ammonia nitrogen removal reached 100% at pH 8.3 or 4. SR-AOP appears to be more advantageous over hydroxyl radical (OH-)-based advanced oxidation processes (HR-AOPs) because OH- almost does not oxidize ammonia. Furthermore, compared with Fenton treatment of the same batch leachate sample, the TPO could achieve a higher COD removal at an identical chemical dose. For example, COD removal was 40% at H_2O_2:2.125COD0 = 2 during Fenton treatment (pH 3), but 91% at S_2O_8~(2-):12COD_0 = 2 during TPO (pH 4). These findings demonstrate that SR-AOP is a promising landfill leachate treatment method.