Nanoarchitectonics with a Membrane-Embedded Electron Shuttle Mimics the Bioenergy Anabolism of Mitochondria.

Enhanced bioenergy anabolism through transmembrane redox reactions in artificial systems remains a great challenge. Here, we explore synthetic electron shuttle to activate transmembrane chemo-enzymatic cascade reactions in a mitochondria-like nanoarchitecture for augmenting bioenergy anabolism. In this nanoarchitecture, dendritic mesoporous silica microparticle as inner compartment possesses higher load capacity of NADH as proton source and allows faster mass transfer. In addition, it permits the stability of the outer compartment ATP synthase-reconstituted proteoliposomes. Like natural enzymes in mitochondrion respiratory chain, small synthetic electron shuttle embedded in lipid bilayer, facilely mediates transmembrane redox reactions to convert NADH into NAD+ and proton. These facilitate enhanced outward proton gradient to drive ATP synthase to rotate for catalytic ATP synthesis with improved performance in a sustainable manner. This present work opens a new avenue to achieve enhanced bioenergy anabolism by utilizing synthetic electron shuttle and tuning inner nanostructures, holding great promise in wide-range ATP-powered bioapplications.