Oxygen‐Rich Carbon Nitrides from an Eutectic Template Strategy Stabilize Ni, Fe Nanosites for Electrocatalytic Oxygen Evolution

<jats:title>Abstract</jats:title><jats:p>Functionalized porous carbons are central to various important applications such as energy storage and conversion. Here, a simple synthetic route to prepare oxygen‐rich carbon nitrides (CNOs) decorated with stable Ni and Fe‐nanosites is demonstrated. The CNOs are prepared via a salt templating method using ribose and adenine as precursors and CaCl<jats:sub>2</jats:sub>·2H<jats:sub>2</jats:sub>O as a template. The formation of supramolecular eutectic complexes between CaCl<jats:sub>2</jats:sub>·2H<jats:sub>2</jats:sub>O and ribose at relatively low temperatures facilitates the formation of a homogeneous starting mixture, promotes the condensation of ribose through the dehydrating effect of CaCl<jats:sub>2</jats:sub>·2H<jats:sub>2</jats:sub>O to covalent frameworks, and finally generates homogeneous CNOs. As a specific of the recipe, the condensation of the precursors at higher temperatures and the removal of water promotes the recrystallization of CaCl<jats:sub>2</jats:sub> (<jats:italic>T</jats:italic> &lt; <jats:italic>T<jats:sub>m</jats:sub></jats:italic> = 772 °C), which then acts as a hard porogen. Due to salt catalysis, CNOs with oxygen and nitrogen contents as high as 12 and 20 wt%, respectively, can be obtained, while heteroatom content stayed about unchanged even at higher temperatures of synthesis, pointing to the extraordinarily high stability of the materials. After decorating Ni and Fe‐nanosites onto the CNOs, the materials exhibit high activity and stability for electrochemical oxygen evolution reaction with an overpotential of 351 mV.</jats:p>