Bandgap‐Broken Fe Spinel Electrocatalyst Enables Integrated Seawater Electrolysis

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Abstract
Despite considerable attention on spinel catalysts in electrocatalysis, achieving their distinct redox activity at the atomic scale for cathodic seawater splitting and anodic wastewater purification represents a huge challenge. In this work, we address this issue by constructing bandgap‐broken Zn─O─Fe─O─Co heteroatomic bonds through the integration of reduced ZnFe 2 O 4 and oxidized CoFe 2 O 4 semiconductors within spinel‐structured Zn x Co 1‐x Fe 2 O 4 . The overlapping conduction and valence bands at Fe 3 d orbitals promote electron redistribution at Fe centers, leading to electron depletion, exposure of empty d orbitals, and modulation of the d‐band center. These electronic modifications enhance the adsorption kinetics of H 2 O in seawater and S 2− species in wastewater through d–p orbital coupling, lowering the energy barriers for the Volmer step in hydrogen evolution reaction and the rate‐limiting *S─*S 2 process in sulfur oxidation reaction. As a result, the rational design enables efficient bifunctional activity, achieving simultaneous seawater splitting and industrial pollutant degradation in a single electrolyzer at an ultralow cell voltage of 1.07 V (10 mA cm −2 ), operable under solar energy. This study provides a fundamental design strategy for bifunctional catalysts toward integrated energy and environmental applications.
Funding Information
  • National Key Research and Development Program of China (2025YFF0516504)
  • National Natural Science Foundation of China (U24A20541)
  • National Natural Science Foundation of China (22308070)
  • National Natural Science Foundation of China (22278094)
  • National Natural Science Foundation of China (W2421038)

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