From Supramolecules to Self‐Templated Porous Carbon and Metal‐Doped Carbon Catalysts

The fabrication of carbon materials usually involves the decomposition of precursors and the reorganization of as‐generated fragments. However, the cleavage of bonds and formation of new bonds at nearly identical spatio‐temporal scale prevent effective yet precise fabrication. Herein, a supramolecular precursor, cucurbit[6]uril, that integrates multiple bonds with distinct bond strengths was proposed to decouple the twin problem of simultaneous bond cleavage and formation, rendering multistage transformations to hierarchical porous carbon (SC) and metal‐doped carbon (SC‐M) materials in a single yet effective pyrolysis step without the assist of any template or additional purification. As a proof‐of‐concept, the as‐fabrication SC‐Fe electrocatalysts realized a Pt/C‐like half‐wave potential of 0.869 V vs. RHE and small Tafel slope of 51.3 mV dec−1 in oxygen reduction reaction. This work not only provides an alternative yet controllable approach to fabricate atomically dispersed electrocatalysts but also sheds a light on the understanding of pyrolysis synthesis and rational design of carbon‐based materials via precursor bond engineering.

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