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An Atomic-Scale Explanation for The High Selectivity Towards Carbon Dioxide Reduction Observed On Liquid Metal Catalysts.
Angew Chem Int Ed Engl
November 2024
MacDiarmid Institute for Advanced Materials and Nanotechnology and Department of Physics, University of Auckland, Private Bag, 92019, Auckland, New Zealand.
The low-temperature liquid metals Ga-In and Ga-Sn have previously showcased >95 % selectivity towards the electrochemical reduction of CO to formate, occuring only when the alloys are melted, not solid. Here, density functional theory molecular dynamics and metadynamics simulations reveal that CO 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.
View Article and Find Full Text PDFDynamic sampling of liquid metal structures for theoretical studies on catalysis.
Chem Sci
December 2023
MacDiarmid Institute for Advanced Materials and Nanotechnology, Department of Physics, University of Auckland Private Bag 92019 Auckland New Zealand
Liquid metals have recently emerged as promising catalysts that can outcompete their solid counterparts for many reactions. Although theoretical modelling is extensively used to improve solid-state catalysts, there is currently no way to capture the interactions of adsorbates with a dynamic liquid metal. We propose a new approach based on molecular dynamics sampling of an adsorbate on a liquid catalyst.
View Article and Find Full Text PDFStructural and electronic changes in Ga-In and Ga-Sn alloys on melting.
Phys Chem Chem Phys
January 2023
MacDiarmid Institute for Advanced Materials and Nanotechnology and Department of Physics, University of Auckland, Private Bag 92019, Auckland, New Zealand.
The melting behaviour of surface slabs of Ga-In and Ga-Sn is studied using periodic density functional theory and molecular dynamics. Analysis of the structure and electronics of the solid and liquid phases gives insight into the properties of these alloys, and why they may act as promising CO reduction catalysts. We report melting points for slabs of hexa-layer Ga-In (386 K) and Ga-Sn (349 K) that are substantially lower than the pure hexa-layer Ga system (433 K), and attribute the difference to the degree to which the dopant (In or Sn) disrupts the layered Ga network.
View Article and Find Full Text PDFSize-dependent trends in the hydrogen evolution activity and electronic structure of MoS nanotubes.
Nanoscale Adv
October 2021
MacDiarmid Institute for Advanced Materials and Nanotechnology, Department of Chemistry, University of Otago P.O. Box 56 Dunedin 9054 New Zealand
The thermodynamics of hydrogen evolution on MoS nanotubes is studied for the first time using periodic density functional theory calculations to obtain hydrogen adsorption free energies (Δ ) on pristine nanotubes and those with S-vacancy defects. Armchair and zigzag MoS nanotubes of different diameters, ranging from 12 to 22 Å, are examined. The H adsorption energy is observed to become more favourable (lower Δ ) as nanotube diameter decreases, with Δ values ranging from 1.
View Article and Find Full Text PDFEnhancing the hydrogen evolution activity of MoS basal planes and edges using tunable carbon-based supports.
Nanoscale
February 2021
MacDiarmid Institute for Advanced Materials and Nanotechnology and Department of Chemistry, University of Otago, P.O. Box 56, Dunedin 9054, New Zealand.
The hydrogen adsorption free energy (ΔG) on the basal plane and edges of MoS is studied using periodic density functional theory, with the catalyst supported by a range of two-dimensional carbon-based materials. Understanding how ΔG can be tuned with support gives insight into MoS as a catalyst for the hydrogen evolution reaction. The supports studied here include graphene oxide materials, heteroatom doped (S, B, and N) graphene, and some insulator materials (hexagonal boron nitride and graphitic carbon nitride).
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