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Updated: Jun 13, 2025

Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
An Atomic-Scale Explanation for The High Selectivity Towards Carbon Dioxide Reduction Observed On Liquid Metal
Charlie Ruffman1, Krista G Steenbergen2, Nicola Gaston1
1MacDiarmid Institute for Advanced Materials and Nanotechnology and Department of Physics, University of Auckland, Private Bag, 92019, Auckland, New Zealand.
Abstract:
The low-temperature liquid metals Ga-In and Ga-Sn have previously showcased >95 % selectivity towards the electrochemical reduction of CO2 to formate, occuring only when the alloys are melted, not solid. Here, density functional theory molecular dynamics and metadynamics simulations reveal that CO2 does not directly adsorb to the Ga-alloy surface, but instead is reduced indirectly by reaction with an adsorbed hydrogen. The reaction barrier is vastly more favourable when this process occurs at In or Sn sites (average: 0.26 eV), than when it occurs on Ga (average: 0.47 eV). However, there is no difference in barrier between solid and liquid surfaces. Instead, we find that Hads is mobile only on the liquid surface, travelling due to the motion of the liquid beneath. This process drives Hads to In/Sn sites, allowing low-barrier CO2 reduction to occur only on the liquid. Therefore, the dynamic motion of liquid metal catalysts can underpin their unique reactivity. The result has far reaching implications for any protonation reaction conducted with a liquid metal catalyst.
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