Universal Sub‐Nanoreactor Strategy for Synthesis of Yolk‐Shell MoS₂ Supported Single Atom Electrocatalysts toward Robust Hydrogen Evolution Reaction

The coordination structure determines the electrocatalytic performances of single atom catalysts (SACs), while it remains a challenge to precisely regulate their spatial location and coordination environment. Herein, we report a universal sub‐nanoreactor strategy for synthesis of yolk‐shell MoS 2 supported single atom electrocatalysts with dual‐anchored microenvironment of vacancy‐enriched MoS 2 and intercalation carbon toward robust hydrogen‐evolution reaction. Theoretical calculations reveal that the “E‐Lock” and “E‐Channel” are conducive to stabilize and activate metal single atoms. A group of SACs is subsequently produced with the assistance of sulfur vacancy and intercalation carbon in the yolk‐shell sub‐nanoreactor. The optimized C−Co−MoS 2 yields the lowest overpotential (η 10 =17 mV) compared with previously reported MoS 2 ‐based electrocatalysts to date, and also affords a 5–9 fold improvement in activity even comparing with those as‐prepared single‐anchored analogues. Theoretical results and in situ characterizations unveil its active center and durability. This work provides a universal pathway to design efficient catalysts for electro‐refinery.