Single atoms and nanoclusters of Fe, Ni, Co, Cu, and Mn are systematically designed and embedded in a well‐defined C1N1‐type material that has internal cavities of ≈0.6 nm based on four N atoms. These N atoms serve as perfect anchoring points for the nucleation of small nanoclusters of different metal natures through the creation of metal‐nitrogen (TM‐N4) bonds. After pyrolysis at 800 °C, TM@CNx‐type structures are obtained, where TM is the transition metal and x < 1. Fe@CNx and Co@CNx are the most promising for oxygen reduction reaction and hydrogen evolution reaction, respectively, with a Pt‐like performance, and Ni@CNx is the most active for oxygen evolution reaction (OER) with an EOER of 1.59 V versus RHE, far outperforming the commercial IrO2 (EOER = 1.72 V). This systematic and benchmarking study can serve as a basis for the future design of advanced multi‐functional electrocatalysts by modulating and combining the metallic nature of nanoclusters and single atoms.

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The study of novel two-dimensional structures for potential applications in photocatalysis or in optoelectronics is a challenging task. In this work, first-principles calculations have been carried out to explore the...