Supramolecular Macrocycle Regulated Single‐Atom MoS2@Co Catalysts for Enhanced Oxygen Evolution Reaction

The development of active water oxidation catalysts for water splitting has stimulated considerable interest. Herein, the design and building of single atom Co sites using a supramolecular tailoring strategy are reported, that is, the introduction of pillar[4]arene[1]quinone (P4A1Q) permits mononuclear Co species stereoelectronically assembled on MoS 2 matrix to construct an atomically dispersed MoS 2 @Co catalyst with modulated local electronic structure, definite chemical environment and enhanced oxygen evolution reaction performance. Theoretical calculations indicate that immsobilized single‐Co sites exhibit an optimized adsorption capability of oxygen‐containing intermediates, endowing the catalyst an excellent electrocatalytic oxygen evolution reaction activity, with a low overpotential of 370 mV at 10 mA cm −2 and a small Tafel slope of 90 mV dec −1 . The extendable potential of this strategy to other electrocatalysts such as MoS 2 @Ni and MoS 2 @Zn, and other applications such as the hydrogen evolution reaction was also demonstrated. This study affords new insights into the rational design of single metal atom systems with enhanced electrocatalytic performance.