The major scientific challenges towards energy dense chemical synthesis using renewable electricity or direct sunlight are hydrocarbon production from CO2 with enough efficiency and, in particular, scale-up to the terawatt level needed for impact on global fuel consumption. Natural photosynthesis provides a successful design concept with minimized non-active components. It is the only technology that generates high energy compounds on a hundred terawatt-scale by accomplishing the most demanding charge transport and primary photochemical transformations on the nanoscale under membrane separation. The recent emergence of ultrathin oxide layers enabled by the techniques of nanoscience, in particular atomic layer deposition, has opened up new pathways for the hierarchical integration of light absorber, catalysts, and membranes. I present the fabrication and photocatalytic performance of a cm2-sized free-standing nanometer-thin multistack of Co3O4/SiO2/light absorber/Cu mechanically supported by mesoporous anodized alumina and silica. Cobalt oxide water oxidation catalyst and Cu CO2 reduction catalyst are separated by a 2 nm thin proton conducting, gas impermeable SiO2 nanomembrane with embedded molecular wires, which enable unidirectional hole transfer from the excited light absorber through the nanomembrane to the water oxidation catalyst. The system is optimized towards photocatalytic performance by varying layer thickness, wire electronic properties, density of light absorbers and catalyst loading using infrared and mass spectroscopy for monitoring. While the planar nanomembrane geometry enables optimization of the wall composition by monitoring photocataytic intermediates and products in the separated compartments, a high surface area morphology is being implemented in the form of a core-shell nanotube array in which each individual nanotube closes the catalytic cycle.

Free-standing ultrathin oxide membrane for photocatalytic CO2 reduction by water under separation of the products

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.