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

利用共晶模板策略制备富氧碳氮化物,可稳定Ni、Fe纳米位点用于电催化析氧反应

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Abstract

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(2) ·2H(2) O as a template. The formation of supramolecular eutectic complexes between CaCl(2) ·2H(2) 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(2) ·2H(2) 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(2) (T < T(m) = 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.

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