Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.237
Publication date: 18th July 2023
The recent emergence of ultrathin oxide layers in catalysis has led to more corrosion-resistant photoelectrodes and enhanced catalytic selectivity – suppressing side reactions and catalyst poisoning [1] Silica nanolayers for example demonstrated enhanced proton transfer [2] and electron transfer [3] across solid-solid interfaces when embedding molecular wires. The nanoscale integration of incompatible catalytic environments of CO2 reduction and H2O oxidation – similar to a thylakoid membrane – can potentially be achieved by such ultrathin oxide layers, provided we can maintain directional electronic and protonic communication across the layer.
Here, we investigate the proton conductivity and O2 impermeability of ultrathin, dense, and amorphous Al2O3 layers and find that the diffusivity of protons is strongly dependent on the flux due to induced morphological changes in the alumina layer over time. Dense amorphous alumina layers were prepared via pulsed laser deposition (PLD; 2.5 nm, 3 nm, and 5 nm) and the porosity was varied via the oxygen background pressure of the chamber. We used electrochemical impedance spectroscopy to determine diffusion coefficients and charge transfer resistances, and complementary electrochemical FT-Infrared reflection-absorption spectroscopy was applied to analyze the dynamic structural changes of alumina over time in-situ (Figure 1b). In fact, we observe that initially, 2.5 nm of alumina can block both protons and oxygen, whereas over time the proton permeation improves while we can exclude dissolution of the Al2O3 layer (Figure 1c)
These discoveries facilitate the integration of incompatible catalytic functions on the nanoscale, thereby opening a new design space for developing macroscale systems. The core–shell nanotube array geometry for developing an artificial photosystem with the goal of placing CO2 reduction inside the tubes and H2O oxidation outside of them is just one among many opportunities to pursue.
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