Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.477
Publication date: 16th December 2024
The water crisis is a major concern at global scale, which underscores the need for alternative freshwater resources. In this context, urban wastewater is one of the main targets to feed regenerated water for many applications, but it faces challenges from persistent pharmaceuticals resistant to conventional treatments. Advanced methods like electrochemical advanced oxidation processes (EAOPs), particularly the electro-Fenton (EF) process, offer a highly promising performance [1]. However, limitations such as narrow pH range and low H2O2 yields must be addressed by developing new electrocatalysts and heterogeneous catalysts.
This work addresses these issues through two innovations: (1) Electrocatalysts for highly selective two-electron oxygen reduction reaction (2e– ORR) to generate H2O2 in situ, and (2) advanced heterogeneous catalysts with enhanced H2O2 activation efficiency.
In EF, 3.0 to 15.0 mM H2O2 is sufficient to purify wastewater [2], making the electrochemical 2e– ORR with a gas-diffusion electrode (GDE) an attractive alternative to the industrialized anthraquinone process to synthesize H2O2. Tin (Sn) exhibits strong O2 adsorption under alkaline conditions [3]; accordingly, Sn-doped carbon materials are demonstrated to have outstanding H2O2 selectivity (98%) and high H2O2 production efficiency at near-neutral pH, with an electron transfer number of 2.04. Nitrogen-doped carbons, optimized for pyrrolic nitrogen content, delivered superior H2O2 yields (reaching 18 mg h–1 cm–2) compared to commercial GDEs.
For H2O2 activation, Cu/NC and FeCu/NC catalysts derived from MOFs exhibited great performance. Cu/NC enabled the effective pollutant mineralization at pH 6–8, being superior to the EF process with soluble Fe2+ at pH 3. The core-shell structure of FeCu/NC minimized metal leaching and extended catalyst lifespan. This brought about an accelerated Fe(II) regeneration, achieving 100% removal of lisinopril within 75 min.
This research shows significant progress in the development of sustainable EF systems, integrating the efficient electrogeneration and activation of H2O2, which allows addressing the problem of pharmaceutical pollutants in wastewater.
The authors are grateful to project PID2022-140378OB-I00, funded by MICIU/AEI/10.13039/501100011033 (Spain) and by ERDF/EU, and to the Ph.D. scholarship awarded to L.Z. (State Scholarship Fund, CSC, China).
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