Interface engineering strategy of a Ti4O7 ceramic membrane via graphene oxide nanoparticles toward efficient electrooxidation of 1,4-dioxane

Abstract

Although Ti₄O₇ ceramic membrane has been recognized as one of the most promising anode materials for electrochemical advanced oxidation process (EAOP), it suffers from relatively low hydroxyl radical (^•OH) production rate and high charge-transfer resistance that restricted its oxidation performance of organic pollutants. Herein, we reported an effective interface engineering strategy to develop a Ti₄O₇ reactive electrochemical membrane (REM) doped by graphene oxide nanoparticles (GONs), GONs@Ti₄O₇ REM, via strong GONs-O-Ti bonds. Results showed that 1% (wt%) GON doping on Ti₄O₇ REM significantly reduced the charge-transfer resistance from 73.87 to 8.42 Ω compared with the pristine Ti₄O₇ REM, and yielded ^•OH at 2.5-2.8 times higher rate. The 1,4-dioxane (1,4-D) oxidation rate in batch experiments by 1%GONs@Ti₄O₇ REM was 1.49×10^-2 min^-1, 2 times higher than that of the pristine Ti₄O₇ REM (7.51×10^-3 min^-1) and similar to that of BDD (1.79×10^-2 min^-1). The 1%GONs@Ti₄O₇ REM exhibited high stability after a polarization test of 90 h at 80 mA/cm², and within 15 consecutive cycles, its oxidation performance was stable (95.1-99.2%) with about 1% of GONs lost on the REM. In addition, REM process can efficiently degrade refractory organic matters in the groundwater and landfill leachate, the total organic carbon was removed by 54.5% with a single-pass REM. A normalized electric energy consumption per log removal of 1,4-D (EE/O) was observed at only 0.2-0.6 kWh/m³. Our results suggested that chemical-bonded interface engineering strategy using GONs can facilitate the EAOP performance of Ti₄O₇ ceramic membrane with outstanding reactivity and stability.

Keywords: Electrochemical advanced oxidation process (EAOP); Graphene nanoparticles; Hydroxyl radical; Reactive electrochemical membrane (REM); Refractory organic matter.