Structure Sensitivity in the Electrocatalytic Reduction of CO2 with Gold Catalysts

Stefano Mezzavilla, Sebastian Horch, Ifan Stephens, Brian Seger, Ib Chorkendorff*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

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Abstract

The understanding of how structural surface features influence electrocatalytic reactions is vital for the development of efficient nanostructured catalysts. Gold is the most active and selective known electrocatalyst for the reduction of CO2 to CO in aqueous electrolytes. Numerous strategies have been proposed to improve its intrinsic activity. Nonetheless, the atomistic knowledge of the nature of the active sites remains elusive. In this work, we systematically investigated the structure sensitivity for the electrocatalytic CO2 reduction with Au single crystals. Reaction kinetics for the formation of CO were strongly dependent on the surface structure: under-coordinated sites, such as the ones present in Au(110) and at the steps of Au(211), show at least 20-fold higher activity than more coordinated configurations (e.g. Au(100)). By selectively poisoning under-coordinated sites with Pb, we confirmed that these are the active sites for CO2 reduction.
Original languageEnglish
JournalAngewandte Chemie International Edition
Volume28
Issue number12
Pages (from-to)3774-3778
Number of pages6
ISSN1433-7851
DOIs
Publication statusPublished - 2019

Keywords

  • CO2 electrolysis
  • Gold
  • Single crystals
  • Structure-sensitivity
  • Poisoning

Cite this

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title = "Structure Sensitivity in the Electrocatalytic Reduction of CO2 with Gold Catalysts",
abstract = "The understanding of how structural surface features influence electrocatalytic reactions is vital for the development of efficient nanostructured catalysts. Gold is the most active and selective known electrocatalyst for the reduction of CO2 to CO in aqueous electrolytes. Numerous strategies have been proposed to improve its intrinsic activity. Nonetheless, the atomistic knowledge of the nature of the active sites remains elusive. In this work, we systematically investigated the structure sensitivity for the electrocatalytic CO2 reduction with Au single crystals. Reaction kinetics for the formation of CO were strongly dependent on the surface structure: under-coordinated sites, such as the ones present in Au(110) and at the steps of Au(211), show at least 20-fold higher activity than more coordinated configurations (e.g. Au(100)). By selectively poisoning under-coordinated sites with Pb, we confirmed that these are the active sites for CO2 reduction.",
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author = "Stefano Mezzavilla and Sebastian Horch and Ifan Stephens and Brian Seger and Ib Chorkendorff",
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Structure Sensitivity in the Electrocatalytic Reduction of CO2 with Gold Catalysts. / Mezzavilla, Stefano; Horch, Sebastian; Stephens, Ifan; Seger, Brian; Chorkendorff, Ib.

In: Angewandte Chemie International Edition, Vol. 28, No. 12, 2019, p. 3774-3778.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Structure Sensitivity in the Electrocatalytic Reduction of CO2 with Gold Catalysts

AU - Mezzavilla, Stefano

AU - Horch, Sebastian

AU - Stephens, Ifan

AU - Seger, Brian

AU - Chorkendorff, Ib

PY - 2019

Y1 - 2019

N2 - The understanding of how structural surface features influence electrocatalytic reactions is vital for the development of efficient nanostructured catalysts. Gold is the most active and selective known electrocatalyst for the reduction of CO2 to CO in aqueous electrolytes. Numerous strategies have been proposed to improve its intrinsic activity. Nonetheless, the atomistic knowledge of the nature of the active sites remains elusive. In this work, we systematically investigated the structure sensitivity for the electrocatalytic CO2 reduction with Au single crystals. Reaction kinetics for the formation of CO were strongly dependent on the surface structure: under-coordinated sites, such as the ones present in Au(110) and at the steps of Au(211), show at least 20-fold higher activity than more coordinated configurations (e.g. Au(100)). By selectively poisoning under-coordinated sites with Pb, we confirmed that these are the active sites for CO2 reduction.

AB - The understanding of how structural surface features influence electrocatalytic reactions is vital for the development of efficient nanostructured catalysts. Gold is the most active and selective known electrocatalyst for the reduction of CO2 to CO in aqueous electrolytes. Numerous strategies have been proposed to improve its intrinsic activity. Nonetheless, the atomistic knowledge of the nature of the active sites remains elusive. In this work, we systematically investigated the structure sensitivity for the electrocatalytic CO2 reduction with Au single crystals. Reaction kinetics for the formation of CO were strongly dependent on the surface structure: under-coordinated sites, such as the ones present in Au(110) and at the steps of Au(211), show at least 20-fold higher activity than more coordinated configurations (e.g. Au(100)). By selectively poisoning under-coordinated sites with Pb, we confirmed that these are the active sites for CO2 reduction.

KW - CO2 electrolysis

KW - Gold

KW - Single crystals

KW - Structure-sensitivity

KW - Poisoning

U2 - 10.1002/anie.201811422

DO - 10.1002/anie.201811422

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VL - 28

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JO - Angewandte Chemie International Edition

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SN - 1433-7851

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ER -