Synergistic Approaches for Enhanced Light-Driven Hydrogen Production: A Membrane-Anchoring Protein-Engineered Biohybrid System with Dual Photosensitizers Strategy

Sunlight-driven hydrogen production provides a sustainable solution for clean energy generation. Despite their potential, extracellular photosensitized biohybrid systems are typically hindered by sluggish electron transfer between semiconductor materials and microorganisms. Herein, we introduce a bioinspired development, the membrane-anchoring protein approach, to overcome this limitation. Using a membrane-anchoring protein incorporated with a TiO 2 binding peptide on engineered E. coli, we establish a proof-of-concept and demonstrate an 81-fold enhancement in electron transfer efficiency and 10.8-fold increase in hydrogen production. Unprecedented insights into the dynamics of the extracellular photosensitized biohybrid interface are revealed herein using methyl viologen as an electron shuttle. Additionally, introducing Eosin Y as a photosensitizer model enhances both the electron source and transfer efficiency, further boosting hydrogen production. The synergistic approach utilizing extracellular and intracellular dual photosensitizers overcomes the limitations of electron transfer, enhances the overall efficiency of the system, and creates a more efficient pathway for light-driven hydrogen production.