Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
DOI: https://doi.org/10.29363/nanoge.nfm.2022.212
Publication date: 11th July 2022
The electrochemical partial oxidation of methane to methanol is a promising approach to the transformation of stranded methane resources into a high-value, easy-to-transport fuel and chemical. The direct transformation of methane to methanol in remote locations requires selective catalysts capable of operating at near ambient temperatures inside a modular device. Over the last decade, transition metal oxides have been shown as potential electrocatalysts for this transformation. However, a comprehensive and systematic study of the dependence of methane activation rates and methanol selectivity on catalyst morphology and experimental operating parameters during testing has not been realized.
In this contribution, we describe an electrochemical method for the deposition of a family of thin-film transition metal (oxy)hydroxides as catalysts for the partial oxidation of methane. CoOx, NiOx, MnOx and CuOx are discovered to be active for the partial oxidation of methane to methanol in a carbonate electrolyte. TiOx and FeOx oxides show no selectivity for methanol at the oxidative potentials tested. Taking CoOx as a prototypical methane partial oxidation electrocatalyst, we systematically study the dependence of activity and methanol selectivity on catalyst film thickness, overpotential, temperature and electrochemical cell hydrodynamics in a gas-tight rotating cylinder electrode cell. Optimal conditions of low catalyst film thickness, intermediate overpotentials and intermediate temperatures are identified to favor methanol accumulation in the electrochemical cell. The rate of transport of methane and methanol in and out of the electrocatalyst surface is also shown to be an important design parameter for future methane to methanol electrochemical cells. Through a combination of control experiments and DFT calculations, we show that the oxidized form of the as-deposited (oxy)hydroxide catalyst films are active for the thermal oxidation of methane to methanol even without the application of a bias potential, demonstrating that high valence transition metal oxides are intrinsically active for the activation and oxidation of methane to methanol at ambient temperatures.
Financial support for this work results from a Scialog program sponsored jointly by Research Corporation for Science Advancement and the Alfred P. Sloan Foundation and includes a grant No. G-2021-14160 by the Alfred P. Sloan Foundation.
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