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Light-Driven Proton Transport Across Liposomal Membranes Enabled by Janus Metal-Organic Layers

36 Pages Posted: 1 Jun 2021 Publication Status: Under Review

See all articles by Huihui Hu

Huihui Hu

Xiamen University - State Key Laboratory of Physical Chemistry of Solid Surfaces

Jieyu Zhu

Xiamen University - State Key Laboratory of Physical Chemistry of Solid Surfaces

Zhiye Wang

Xiamen University - State Key Laboratory of Physical Chemistry of Solid Surfaces

Liulin Yang

Xiamen University - State Key Laboratory of Physical Chemistry of Solid Surfaces

Wenbin Lin

University of Chicago - Department of Chemistry

Cheng Wang

Xiamen University - State Key Laboratory of Physical Chemistry of Solid Surfaces

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Abstract

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 generation of a proton gradient via directional proton transport. Here we report a light-driven proton pump based on two-dimensional, porphyrin-based Janus metal-organic layers (Janus-MOLs) embedded in liposomes. We developed a microemulsion-based method to functionalize the Janus-MOLs with carboxyquinone on one side and Acitretin on the other side. By attaching the Janus-MOLs to liposome surfaces, we obtained a mimic to photosynthetic bacteria. 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·) in the lipid bilayer to produce a concentration gradient of quinone-based species. Owing to different pKa values of HQ+ and HQ ·, these redox reactions trigger proton transport across the membrane to create a pH gradient, which drives ATP production by CF0F1-ATP synthase in a similar fashion as photosynthetic bacteria.

Keywords: Proton Pump; Light-driven Proton Transport; ATP Synthesis; Metal-Organic Layer; Mimicking Bacteria Photosynthesis

Suggested Citation

Hu, Huihui and Zhu, Jieyu and Wang, Zhiye and Yang, Liulin and Lin, Wenbin and Wang, Cheng, Light-Driven Proton Transport Across Liposomal Membranes Enabled by Janus Metal-Organic Layers. Available at SSRN: https://ssrn.com/abstract=3858057 or http://dx.doi.org/10.2139/ssrn.3858057
This version of the paper has not been formally peer reviewed.

Huihui Hu

Xiamen University - State Key Laboratory of Physical Chemistry of Solid Surfaces

No. 422, South Siming Road
Xiamen, Fujian 361005
China

Jieyu Zhu

Xiamen University - State Key Laboratory of Physical Chemistry of Solid Surfaces ( email )

Xiamen, 361005
China

Zhiye Wang

Xiamen University - State Key Laboratory of Physical Chemistry of Solid Surfaces ( email )

Xiamen, 361005
China

Liulin Yang

Xiamen University - State Key Laboratory of Physical Chemistry of Solid Surfaces ( email )

Xiamen, 361005
China

Wenbin Lin

University of Chicago - Department of Chemistry ( email )

1101 East 58th Street
Chicago, IL 60637
United States

Cheng Wang (Contact Author)

Xiamen University - State Key Laboratory of Physical Chemistry of Solid Surfaces ( email )

No. 422, South Siming Road
Xiamen, Fujian 361005
China

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