Abstract
<h2>Summary</h2> Photo-generation of a proton gradient over a lipid bilayer is of interest due to its essential role in photosynthetic bacteria. Membrane asymmetry is key to the proton gradient generation via directional proton transport. Here, we report a light-driven proton pump based on two-dimensional, porphyrin-based Janus metal-organic layers (Janus-MOLs). The Janus-MOL, functionalized with carboxyquinone on one side and Acitretin on the other via a microemulsion-based method, was attached to liposome surface. Upon photoexcitation, the porphyrins initiate electron and hole transfers to carboxyquinone and Acitretin, respectively, which undergo redox reactions with freely diffusing quinone (Q)/hydrosemiquinone (HQ<sup>·</sup>) in the lipid bilayer to produce a concentration gradient of quinone-based species. Owing to different pKa values of HQ<sup>+</sup> and HQ<sup>·</sup>, these redox reactions trigger proton transport across the membrane to create a pH gradient, which drives ATP production by CF<sub>o</sub>F<sub>1</sub>-ATP synthase in a similar fashion as photosynthetic bacteria.
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