Effects of gas saturation and sparging on sonochemical oxidation activity in open and closed systems, Part I: H2O2 generation

Cavitational/sonochemical activity can be significantly enhanced or reduced depending on the gases dissolved in the liquid. Although many researchers have suggested the order of importance of dissolved gas conditions that affect the degree of sonoluminescence (SL), sonochemiluminescence (SCL), and compound degradation, the most suitable gas condition for sonochemical oxidation reactions is currently unknown. In this study (Part I), the effects of gas saturation and sparging on the generation of H2O2 were investigated in a 28-kHz sonoreactor system. Four gas modes, saturation/closed, saturation/open, sparging/closed, and sparging/open, were applied to Ar, O2, N2, and binary gas mixtures. The change in dissolved oxygen (DO) concentration during ultrasonic irradiation was measured and was used as an indicator of whether the gaseous exchange between liquid and air altered the gas content of the liquid. Considerable difference in the DO concentration was observed for the gas saturation/open mode, ranging from -11.5 mg/L (O2 100 %) to +4.3 mg/L (N2 100 %), while no significant difference was observed in the other gas modes. The change in the gas content significantly reduced the linearity for H2O2 generation, which followed pseudo-zero-order kinetics, and either positively or negatively affected H2O2 generation. Ar:O2 (75:25) and Ar:O2 (50:50) resulted in the highest and second-highest H2O2 generation for both gas saturation and sparging, respectively. In addition, gas sparging resulted in much higher H2O2 generation for all gas conditions compared to gas saturation; this was because of the significant change in the cavitational active zone and concentrated ultrasonic energy, which formed a bulb-shaped active zone, especially for the Ar/O2 mixtures adjacent to the transducer at the bottom. The sparging flow rate and position also significantly affected H2O2 generation; the highest H2O2 generation was obtained when the sparger was placed at the bottom adjacent to the transducer, with a flow rate of 3 L/min. In Part II, the generation of nitrogen oxides, including nitrite (NO2-) and nitrate (NO3-), was investigated using the same ultrasonic system with three gas modes: saturation/open, saturation/closed, and sparging/closed.