Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.227
Publication date: 18th December 2023
The urgent need for large-scale renewable energy storage and carbon mitigation strategies calls for efficient methods of converting carbon dioxide (CO2) into valuable hydrocarbon fuels1. Among these, methane (CH4) holds particular promise due to its high energy density and compatibility with existing infrastructure. Electrochemical CO2 reduction (CO2R) to CH4 offers a direct pathway to decarbonize natural gas, but practical applications require high current densities, selectivity, and energy efficiency [1,2].
In this study, we present a novel approach to enhance CH4 production via CO2R in aqueous bicarbonate systems [3]. Our research addresses the limitations of previous systems and introduces a paradigm shift in CO2 electroreduction. We leverage the benefits of large-pore Cu electrodes, which facilitate the transport of dissolved CO2 and promote efficient bicarbonate conversion into CO2. This architectural innovation results in high local CO2 concentrations crucial for CH4 selectivity.
Furthermore, we introduce an in-situ Cu activation strategy achieved through alternating current operation. This activation method not only generates, but also maintains a highly selective Cu catalyst surface, favoring CH4 production over hydrogen evolution. Our aqueous-fed system achieves remarkable CH4 Faradaic efficiencies, exceeding 70% across a wide current density range (100–750 mA cm-2), and maintains stability for at least 12 hours at 500 mA cm-2.
Importantly, our system also demonstrates the highest CH4 product concentration, compared to previous CO2-to-CH4 systems. These findings open new avenues for the large-scale production of CH4 via CO2R, with implications for renewable energy storage and the reduction of greenhouse gas emissions. We believe our innovative approach paves the way for practical and sustainable CH4 production from CO2, contributing to the global effort to combat climate change.
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