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Molecular tunability of surface-functionalized metal nanocrystals for selective electrochemical CO2 reduction

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Abstract

Organic ligands are used in homogeneous catalysis to tune the metal center reactivity; in contrast, clean surfaces are usually preferred in heterogeneous catalysis. Herein, we demonstrate the potential of a molecular chemistry approach to develop efficient and selective heterogeneous catalysts in the electrochemical CO2 reduction reaction (CO2RR). We have tailor-made imidazolium ligands to promote the CO2RR at the surface of hybrid organic/inorganic electrode materials. We used silver nanocrystals for the inorganic component to obtain fundamental insights into the delicate tuning of the surface chemistry offered by these ligands. We reveal that modifying the electronic properties of the metal surface with anchor groups along with the solid/liquid interface with tail groups is crucial in obtaining selectivities (above 90% FE for CO), which are higher than the non-functionalized Ag nanocrystals. We also show that there is a unique dependency of the CO2RR selectivity on the length of the hydrocarbon tail of these ligands, offering a new way to tune the interactions between the metal surface with the electrolyte and reactants.

Graphical abstract: Molecular tunability of surface-functionalized metal nanocrystals for selective electrochemical CO2 reduction

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Publication details

The article was received on 03 Sep 2019, accepted on 19 Sep 2019 and first published on 23 Sep 2019


Article type: Edge Article
DOI: 10.1039/C9SC04439F
Chem. Sci., 2019, Advance Article
  • Open access: Creative Commons BY-NC license
    All publication charges for this article have been paid for by the Royal Society of Chemistry

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    Molecular tunability of surface-functionalized metal nanocrystals for selective electrochemical CO2 reduction

    J. R. Pankhurst, Y. T. Guntern, M. Mensi and R. Buonsanti, Chem. Sci., 2019, Advance Article , DOI: 10.1039/C9SC04439F

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