Flow effects on phenol degradation and sonoluminescence at different ultrasonic frequencies

Ultrason Sonochem. 2020 May:63:104892. doi: 10.1016/j.ultsonch.2019.104892. Epub 2019 Nov 25.

Abstract

Current literature shows a direct correlation between the sonochemical (SC) process of iodide oxidation and the degradation of phenol solution. This implies phenol degradation occurs primarily via oxidisation at the bubble surface. There is no work at present which considers the effect of fluid flow on the degradation process. In this work, parametric analysis of the degradation of 0.1 mM phenol solution and iodide dosimetry under flow conditions was undertaken to determine the effect of flow. Frequencies of 44, 300 and 1000 kHz and flow rates of 0, 24, 228 and 626 mL/min were applied with variation of power input, air concentration, and surface stabilisation. Phenol degradation was analysed using the 4-aminoantipyrine (4-AAP) method, and sonoluminescence (SL) images were evaluated for 0.1, 20 and 60 mM phenol solutions. Flow, at all frequencies under certain conditions, could augment phenol degradation. At 300 kHz there was excellent correlation between phenol degradation and dosimetry indicating a SC process, here flow acted to increase bubble transience, fragmentation and radical transfer to solution. At 300 kHz, although oxidation is the primary phenol degradation mechanism, it is limited, attributed to degradation intermediates which reduce OH radical availability and bubble collapse intensity. For 44 and 1000 kHz there was poor correlation between the two SC processes. At 44 kHz (0.01 mM), there was little to suggest high levels of intermediate production, therefore it was theorised that under more transient bubble conditions additional pyrolytic degradation occurs inside the bubbles via diffusion/nanodroplet injection mechanisms. At 1000 kHz, phenol degradation was maximised above all other systems attributed to increased numbers of active bubbles combined with the nature of the ultrasonic field. SL quenching, by phenol, was reduced in flow systems for the 20 and 60 mM phenol solutions. Here, where the standing wave field was reinforced, and bubble localisation increased, flow and the intrinsic properties of phenol acted to reduce coalescence/clustering. Further, at these higher concentrations, and in flow conditions, the accumulation of volatile phenol degradation products inside the bubbles are likely reduced leading to an increase SL.