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Metal-free graphdiyne doped with sp-hybridized boron and nitrogen atoms at acetylenic sites for high-efficiency electroreduction of CO2 to CH4 and C2H4

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Abstract

Carbon dioxide electrochemical reduction (CO2ER) to useful fuels and chemicals under ambient conditions provides an intriguing picture for resolving energy security and environmental issues, which mainly relies on metal-based electrocatalysts, but the emerging doped carbon-based materials hold great promise as metal-free alternatives. Here, by means of density functional theory (DFT) computations, the potential of the experimentally available doped graphdiyne (GDY) with boron (B) and nitrogen (N) atoms as the metal-free CO2ER electrocatalyst was systematically explored. Our results revealed that these doped GDYs exhibit extremely high stability due to their high cohesive energies. Interestingly, the GDYs doped with sp-hybridized B and N at their acetylenic sites exhibit quite high-electrocatalytic activity for the conversion of CO2 to CH4 and (especially) C2H4 with a low limiting potential of about −0.60 V, which is attributed to their high electrical conductivity, preferable catalytic sites (sp-hybridized dopant), and low free energy for CO2 activation. Thus, by carefully tailoring the dopant sites of B and N atoms, the doped GDY can be utilized as the metal-free CO2ER catalyst with high-efficiency for the production of C1 and C2 species, which provides a new avenue to advance sustainable CO2 conversion.

Graphical abstract: Metal-free graphdiyne doped with sp-hybridized boron and nitrogen atoms at acetylenic sites for high-efficiency electroreduction of CO2 to CH4 and C2H4

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Publication details

The article was received on 07 Dec 2018, accepted on 21 Jan 2019 and first published on 22 Jan 2019


Article type: Paper
DOI: 10.1039/C8TA11825F
Citation: J. Mater. Chem. A, 2019, Advance Article

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    Metal-free graphdiyne doped with sp-hybridized boron and nitrogen atoms at acetylenic sites for high-efficiency electroreduction of CO2 to CH4 and C2H4

    J. Zhao, Z. Chen and J. Zhao, J. Mater. Chem. A, 2019, Advance Article , DOI: 10.1039/C8TA11825F

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