Atomic H*-mediated electrochemical reduction of bromate by a facile Ti/Pd@MXene filter electrode

J Hazard Mater. 2024 Nov 20:482:136598. doi: 10.1016/j.jhazmat.2024.136598. Online ahead of print.

Abstract

Bromate (BrO3-) is a common by-product of advanced oxidation water treatment processes. In this study, a catalyst combining MXene and Pd was synthesized to eliminate BrO3- by electrochemical reduction in flow-through mode. The fabricated Ti/Pd@MXene filter showed superior activity for BrO3- reduction compared with Ti/MXene filter. A satisfactory BrO3- removal performance by Ti/Pd@MXene filter was obtained at pH values of 5-7 with a current density of 1.0-2.5 mA·cm-2. The mechanism explored by quenching experiments and EPR analysis demonstrated that atomic hydrogen (H*)-mediated reduction was dominant in the Ti/Pd@MXene filter system and contributed to 84.2 % of the BrO3- removal, which was greater than that of Ti (7.1 %) and Ti/MXene (43.9 %). DFT calculations revealed the introduction of Pd nanoparticles on MXene lowered the energy barrier for generating H* from OH* -H* , thus boosting H* formation. Furthermore, the Ti/Pd@MXene filter had favorable stability and applicability, and nearly 90 % of BrO3- could be eliminated in different water matrices. Moreover, energy consumption of the Ti/Pd@MXene filter was more competitive than that previously reported (0.348 kWh·mmol-1), especially for high BrO3- removal (≥75 %). This work highlighted an effective flow-through electrocatalytic filter to induce H* -mediated electrochemical reduction of BrO3-.

Keywords: Atomic hydrogen; Flow-through; Indirect reduction; Pd nanoparticles.