Work

Direct Synthesis of Pure Aqueous H 2 O 2 Solutions Catalyzed by C 60 -Buffered Proton–Electron Transfer on Palladium Adatoms

Year: 2026

Type: article

Abstract: The proton–electron transfer (PET) reaction is a fundamental pathway in redox catalysis that drives critical processes from enzymatic reactions to sustainable fuel generation. Yet its efficient implementation in heterogeneous systems often necessitates liquid-phase molecular mediators, which limit sustainability and simplicity. Direct H 2 O 2 synthesis exemplifies this challenge, where high selectivity conventionally requires organic solvents to mediate PET and suppress side reactions. Herein, this limitation is mitigated by employing C 60 as a solid-state replacement for molecular mediators; we report a palladium adatom catalyst on C 60 that enables direct H 2 O 2 synthesis in pure water, achieving an exceptional rate of 150 mol kg cat –1 h –1 with 90% selectivity and a record product concentration of 0.56 wt %. The benchmark performance stems from a “C 60 -buffered PET” mechanism, wherein C 60 dynamically regulates both electron density and proton/hydrogen species flux, which cooperates with the selective palladium adatom site to inhibit both O–O bond cleavage and overhydrogenation.

Source: Journal of the American Chemical Society

DOI: 10.1021/jacs.6c04486