Soil water

Nanotechnology

Organic chemistry

Electrophoretic deposition

Coating

Rational design

Leaching (pedology)

Composite number

Engineering

Catalysis

Carbon fibers

Physical chemistry

Soil science

Composite material

Chemistry

Metallurgy

Materials science

Oxide

Graphene

Cathode

Environmental science

Chemical engineering

ACS Catalysis

Maintaining a long-term service life of catalytic materials under the established configuration and design concept is a key focus in catalytic process research and development, especially for iron-functionalized cathode-based heterogeneous electro-Fenton (EF) processes operated under harsh conditions. Herein, a versatile and robust encapsulation engineering strategy is proposed based on the concept of tightly covering the surface of conventional iron-functionalized cathodes with an ultrathin carbon layer to significantly improve the stability of composite cathodes without causing activity loss. Taking carbon cloth-supported iron oxychloride (FeOCl/CC) as a model cathode catalyst, it was successfully encapsulated in a reduced graphene oxide protective shell (FeOCl/CC@rGO) using an electrophoretic deposition method, thereby achieving high stability due to negligible iron leaching (only 0.57% of FeOCl/CC), while maintaining almost unaffected activity due to electron penetration effect. Experimental analysis of the structure–activity relationship and theoretical calculations were used to establish the underlying molecular mechanism of electron penetration-triggered H2O2 activation on the outermost surface of rGO. This study uses an effective approach to overcome the activity–stability trade-off of integrated cathodes in heterogeneous EF processes, providing theoretical guidance for the rational design of high-performance cathodes with an encapsulated structure.

Overcoming the Activity–Stability Trade-Off in Heterogeneous Electro-Fenton Catalysis: Encapsulating Carbon Cloth-Supported Iron Oxychloride within Graphitic Layers