Efficient Synthesis and Catalytic Performance Tuning of High-Entropy Alloys Using a Weaving Strategy

High-entropy alloys (HEAs) have garnered considerable interest for their exceptional properties, notably in catalysis, owing to their multiple active sites and synergistic metal interactions. High-entropy metal-organic frameworks (HE-MOFs) have emerged as promising precursors for the synthesis of diverse HEAs. However, conventional approaches to synthesizing HE-MOFs rely primarily on increasing metal ion diversity within the MOF nodes, often leading to complex and poorly controlled reaction kinetics. In this work, we present a novel weaving strategy that incorporates the pre-synthesis of metal-ligand complexes (MLs) as modular building blocks to overcome the intricate coordination dynamics associated with multiple metal ions and ligands. By designing a series of ML "threads" and precisely controlling their stoichiometry and combination, we successfully fabricate HE-MOFs incorporating cerium oxide clusters as structural nodes. Subsequent carbonization and reduction convert these HE-MOFs into CeO₂/C-supported alloys or HEAs with finely adjustable metal contents and tunable catalytic properties. A dye-sensitized photocatalytic hydrogen evolution system revealed that the optimized HEAs(10L)/CeO₂/C catalyst exhibits a hydrogen evolution rate of 13.4 mmol g^-1 h^-1. This pioneering method permits atomic-level control over the metal composition of HEAs, ensuring a broad range of metal ions are homogeneously distributed and enabling the rational design of highly efficient catalytic systems.