Low-Temperature Removal of Refractory Organic Pollutants by Electrochemical Oxidation: Role of Interfacial Joule Heating Effect.

Low temperature presents a challenge to wastewater treatment in the winters of cold regions. In the electrochemical oxidation (EO) process, the interfacial Joule heating (IJH) effect results in interfacial temperature higher than that of bulk electrolytes, which would alleviate the negative impact of low water temperature on organic oxidation occurring within the boundary layer of the anode. This study investigated the electrochemical oxidation of the representative recalcitrant organic pollutant, i.e., phenol, p-chlorophenol (p-CP), and 2,4-dichlorophenoxyacetic acid (2,4-D) on titanium suboxide (TiSO) anode at a low water temperature (8.5 ± 1 °C). At a low current density of 2 mA cm-2, the IJH effect was insignificant and thus had a slight impact on interfacial temperature, leading to a low-efficiency and incomplete organic removal via direct electron transfer (DET) oxidation. Increasing the current density to 20 mA cm-2 promoted the working up of the IJH effect and thus resulted in a dramatic increase in the interfacial temperature from 8.1 to 38.7 °C. This almost eliminated the negative impact of low temperature on the abatement of organic pollutants as though the low temperature of the bulk solution did not interact with interfacial reactions at all. This was indicated by the oxidation rates of 0.158 min-1 (phenol), 0.084 min-1 (p-CP), and 0.070 min-1 (2.4-D) at a temperature of 8.5 ± 1 °C, the values being almost comparable to that obtained at room temperature (23.5 ± 1 °C). Both theoretical and experimental results demonstrated that the extent to which the low- and room-temperature cases deviated from each other was positively correlated with the activation energy of organic pollutants when reacting with •OH. The improvement of organic oxidation at low temperature should result from the compensation of the IJH effect, giving rise to higher •OH reactivity, more activated organic molecules, and enhanced mass transfer. This study may prompt new possibilities to develop an IJH effect-based electrochemical manner for decentralized water decontamination in cold regions.