Catalytic membrane electrode with Co3O4 nanoarrays for simultaneous recovery of water and generation of hydrogen from wastewater

Tremendous research efforts have been devoted to new methods of water decontamination and water splitting at low cost and less energy consumption. Herein, we developed a robust electrochemical strategy with an efficient membrane electrode to remove refractory organic pollutants and simultaneously produce pure hydrogen in wastewater. Firstly, the membrane anode was constructed with a three-dimensional (3D) nanoneedle array of Co3O4 and Ti membrane, exhibiting superior degradation of phenol and dye with Na2SO4 as the electrolyte in a conventional electrocatalytic membrane reactor (ECMR). For the phenol degradation, ≥99% removal efficiency of phenol, 99.5% chemical oxygen demand (COD) removal rate, 92.5% total organic carbon (TOC) removal rate, 88.7% current efficiency and 0.061 kW h (g COD)−1 energy consumption can be obtained. For the dye degradation, ≥99% decolor efficiency and 95.2% COD removal rate, 87.6% TOC removal rate, 82.1% current efficiency and 0.12 kW h (g COD)−1 energy consumption can be achieved. The obtained membrane electrode can provide more active CoOOH sites, dramatically increase the electric fields and overcome mass transfer limitation in a flow-through configuration, thereby significantly enhance the catalytic performance. Finally, we designed a H-type ECMR with the proton exchange membrane (PEM) as the separator for pure H2 production, i.e., PEM-ECMR, demonstrating superior degradation performance of phenol and dye, stable production of high-purity hydrogen (11–15 mL h−1), and excellent long-term stability (100 days) and low voltage input (below 3.0 V). This work demonstrates a promising pathway towards reducing cost and energy consumption for water decontamination and simultaneous hydrogen production.