Tailoring the Selective Oxidation of Hydroxyl-Containing Compounds via Precisely Tuning the Hydrogen-Bond Strength of Catalyst H-Bond Acceptors.

ABSTRACT: The unique performance of the enzyme is mainly achieved via weak interactions between the "outer coordination sphere" and the substrate. Inspired by this process, we developed 3D encapsulated-structure catalysts with hydrogen-bond engineering on the shell, which mimics the "outer coordination sphere" of an enzyme. Various hydrogen bond acceptors (C=O, S=O, and N-O groups) are imparted in the shell. Concentration-dependent ¹H NMR, inverse-phase gas Chromatography (IGC) measurements, and DFT calculations underscore that the hydrogen bond strength between the acceptor groups and alcohol follows the order of C=O < S=O < N-O. The hydroxyl compound oxidation rate vs the hydrogen bond strength follows a volcano behavior, reminiscent of Sabatier's principle. The performance variation am

SUBMITTER: Feng X 

PROVIDER: S-EPMC11938016 | biostudies-literature | 2025 Mar

REPOSITORIES: biostudies-literature