Copper-Modified Covalent Triazine Frameworks as Non-Noble-Metal Electrocatalysts for Oxygen Reduction

The electrochemical oxygen reduction reaction (ORR) is an important cathode reaction of various types of fuel cells. The development of electrocatalysts composed only of abundant elements is a key goal because currently only platinum is a suitable catalyst for ORR. Herein, we synthesized copper‐modified covalent triazine frameworks (CTF) hybridized with carbon nanoparticles (Cu‐CTF/CPs) as efficient electrocatalysts for the ORR in neutral solutions. The ORR onset potential of the synthesized Cu‐CTF/CP was 810 mV versus the reversible hydrogen electrode (RHE; pH 7), the highest reported value at neutral pH for synthetic Cu‐based electrocatalysts. Cu‐CTF/CP also displayed higher stability than a Cu‐based molecular complex at neutral pH during the ORR, a property that was likely as a result of the covalently cross‐linked structure of CTF. This work may provide a new platform for the synthesis of durable non‐noble‐metal electrocatalysts for various target reactions. Stable and efficient: The pores of covalent triazine frameworks hybridized with carbon nanoparticles were functionalized with Cu atoms by coordination to N atoms. The material functions as an efficient electrocatalyst for oxygen reduction reactions (ORR) in neutral solutions. The catalyst exhibited higher stability compared to other Cu‐based organometallic catalysts as a result of the rigid network of covalent bonds in the framework.