Park, Joon Woo Choi, Woong Noh, Juhwan Park, Woonghyeon Gu, Geun Ho Park, Jonghyeok Jung, Yousung Song, Hyunjoon 2024-01-19T12:33:50Z 2024-01-19T12:33:50Z 2022-04-05 2022-02 1944-8244 https://pubs.kist.re.kr/handle/201004/115665 Alloy formation is an advanced approach to improve desired properties that the monoelements cannot achieve. Alloys are usually designed to tailor intrinsic natures or induce synergistic effects by combining materials with distinct properties. Indeed, unprecedented properties have emerged in many cases, superior to a simple sum of pure elements. Here, we present Au-Ag alloy nanostructures with prominent catalytic properties in an electrochemical carbon dioxide reduction reaction (eCO(2)RR). The Au-Ag hollow nanocubes are prepared by galvanic replacement of Au on Ag nanocubes. When the Au-to-Ag ratio is 1:1 (Au1Ag1), the alloy hollow nanocubes exhibit maximum Faradaic efficiencies of CO production in a wide potential range and high mass activity and CO current density superior to those of the bare metals. In particular, overpotentials are estimated to be similar to or lower than that of the Au catalyst under various standard metrics. Density functional theory calculations, machine learning, and a statistical consideration demonstrate that the optimal configuration of the *COOH intermediate is a bidentate coordination structure where C binds to Au and O binds to Ag. This active Au-Ag neighboring configuration has a maximum population and enhanced intrinsic catalytic activity on the Au1Ag1 surface among other Au-to-Ag compositions, in good agreement with the experimental results. Further application of Au1Ag1 to a membrane electrode assembly cell at neutral conditions shows enhanced CO Faradaic efficiency and current densities compared to Au or Ag nanocubes, indicating the possible extension of Au- Ag alloys to larger electrochemical systems. These results give a new insight into the synergistic roles of Au and Ag in the eCO(2)RR and offer a fresh direction toward a rational design of bimetallic catalysts at a practical scale. English American Chemical Society Bimetallic Gold-Silver Nanostructures Drive Low Overpotentials for Electrochemical Carbon Dioxide Reduction Article 10.1021/acsami.1c20852 1 ACS Applied Materials & Interfaces, v.14, no.5, pp.6604 - 6614 ACS Applied Materials & Interfaces 14 5 6604 6614 N scie scopus 000758115300001 2-s2.0-85124147927 Nanoscience & Nanotechnology Materials Science, Multidisciplinary Science & Technology - Other Topics Materials Science Article; Early Access CO2 REDUCTION ELECTROCATALYTIC REDUCTION UNDERPOTENTIAL DEPOSITION AG NANOCUBES ELECTROREDUCTION NANOPARTICLES CATALYSTS CONVERSION METHANE ALLOYS machine learning electrochemical carbon dioxide reduction galvanic replacement random alloy gas diffusion electrode membrane electrode assembly