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

Abstract

Abstract 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 CeO 2 /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)/CeO 2 /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.