4.6 Article

Graphdiyne enables Cu nanoparticles for highly selective electroreduction of CO2 to formate

Journal

2D MATERIALS
Volume 8, Issue 4, Pages -

Publisher

IOP PUBLISHING LTD
DOI: 10.1088/2053-1583/ac217b

Keywords

graphdiyne; copper; electrocatalysis; CO2 reduction; formate

Funding

  1. National Natural Science Foundation of China [21790052, 21931007]
  2. National Key R&D Program of China [2017YFA0700104]
  3. 111 Project of China [D17003]

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The study presents a novel Cu/pyrenyl-graphdiyne composite catalyst for efficient conversion of CO2 to formate in electroreduction, exhibiting excellent selectivity and activity achieved through the combined use of metallic Cu nanoparticles and 2D Pyr-GDY support.
Undoped Cu nanoparticles (NPs) generally show poor selectivity and activity for electroreduction of CO2 to formate due to hard desorption of HCOO* intermediate on Cu site. Here we report a Cu/pyrenyl-graphdiyne (Pyr-GDY) composite catalyst, in which Cu2O and CuO NPs were in-situ formed and embedded in the matrix of a two-dimensional (2D) Pyr-GDY, during the synthesis of 2D Pyr-GDY using monolayer graphene covered Cu foil as a template, and copper acetate as a coupling catalyst. Cu2O and CuO NPs in Cu/Pyr-GDY can be electrochemically reduced to cubic metallic CuNPs to get Cu/Pyr-GDY-R electrocatalyst, with the average size of metallic Cu NPs being 42 nm. The Cu/Pyr-GDY-R on Cu foil can be directly used as a highly efficient electrocatalyst for CO2-to-formate conversion in a CO2-saturated 0.1 M KHCO3 electrolyte, with a formate Faradaic efficiency (FEformate) as high as 95% (at -1.2 V vs reversible hydrogen electrode), far superior to that of Pyr-GDY-free Cu NPs (with a FEformate of only 29%). The key reaction intermediate of HCOO* during CO2-to-formate conversion was identified by in situ Raman spectroscopy. The results of density functional theory calculations revealed that the Pyr-GDY support can decrease the reaction free energy for the adsorption of HCOO* on Cu site, due to the electron transfer from metallic Cu NPs to conjugated diacetylene groups in 2D Pyr-GDY support, which leads to the high selectivity for formate over hydrogen production.

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