Tuning Thiol-Based Self-Assembled Monolayer Chemistry on a Gold Surface towards the Synthesis of Biochemical Fuel.

A proton gradient across a lipid membrane is required for the production of biochemical fuel. Much effort has been devoted to reactions involving proton production in biomimetic assembled architectures under mild conditions. Herein, we explored thiol-based self-assembled monolayer chemistry on a naked gold surface for the production of biochemical fuel. Protons are generated when alkanethiols self-assemble on a gold surface, and the proton yield can be tuned by the choice of thiol and by variation of the procedure used for the deposition of gold. Consequently, the proton gradient across a lipid membrane above the gold surface can be modulated to vary the production rate of biochemical fuel performed by lipid-embedded motor proteins. Our work presents evidence that a simple and efficient abiotic chemical reaction in a well-defined biohybrid system can convert unnatural chemicals, namely alkanethiols, into bioenergy molecules, a finding that has a great potential in biofuel-driven catalysis and devices.