Gram‐Scale Synthesized Two‐Dimensional VSe2 and SnSe2 for Ultrahigh Electrocatalytic Sulfion Recycling

Abstract The electrocatalytic sulfion (S 2− ) recycling and hydrogen (H 2 ) evolution play indispensable roles in converting waste into sustainable energy and boosting hydrogen economy. However, the development of such promising technologies is hindered by the lack of electrocatalysts with low‐cost, high‐efficient, and robust stability. 2D VSe 2 and SnSe 2 hold great application potentials in the energy‐related fields yet face daunting challenges in terms of large‐scale synthesis. Herein, a gram‐scale and high‐yield strategy is designed with tetradecylamine (TDA) assistance for synthesizing 2D VSe 2 and SnSe 2 . The cooperativity of TDA with V 4+ (Sn 4+ ) cations and its stabilization to (100) facets of products contribute to the formation of ultrathin VSe 2 nanosheets with abundant wrinkles and SnSe 2 nanoflowers with hierarchical structures, which deliver excellent hydrogen evolution reaction and oxygen evolution reaction performances. Significantly, a record‐breaking sulfion oxidation reaction efficiency in 2D VSe 2 is uncovered, and the current density is one order of magnitude larger than that of commercial Pt/C catalyst. This work presents a significant breakthrough for scalable synthesize 2D electrocatalysts and provides a new paradigm for sustainable hydrogen generation and water purification.