4.8 Article

Self-reconstruction of paddle-wheel copper-node to facilitate the photocatalytic CO2 reduction to ethane

Journal

APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 310, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apcatb.2022.121320

Keywords

Carbon dioxide fixation; Photocatalysis; Metal-organic framework; Reconstruction; Hydrocarbons

Funding

  1. National Key Research and Development Program of China [2020YFA0710303, 2020YFC1808401]
  2. National Natural Science Foundation of China [22076193, 21827809]
  3. Strategic Priority Research Program B of the Chinese Academy of Sciences [XDB36000000]

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This study successfully obtained high-value-added C2+ hydrocarbons by reducing CO2 using a hybrid photocatalyst. The hybrid photocatalyst exhibited excellent selectivity and efficiency, with the node sites of the two-dimensional MOF playing a critical role in the generation of C2H6.
Obtaining high-value-added products like C2+ hydrocarbons from CO2 reduction in a photocatalytic system has always remained a great challenge. Herein we fabricated a pi-pi stacking hybrid photocatalyst by combining two two-dimensional (2D) materials of g-C3N4 and Cu-porphyrin metal-organic framework (MOF). This hybrid photocatalyst exhibited the excellent capability to reduce CO(2 )into C2H6 in a selectivity of 44% and the selec-tivity of total hydrocarbons (C2H6 and CH4) was as high as 71%, as one of the best performances among the reported photocatalytic systems. The node sites of 2D-MOF were identified to be critical for the generation of C2H6, and a self-reconstruction during photocatalysis was clarified: the initial paddle-wheel Cu-2(II)(COO)(4) node was reconstructed to the partially reduced Cu-2(1+delta)(COO)(3). Such reconstruction strengthened the trapping of in -situ generated CO and the synergistic action of the dual-Cu-site, therefore, achieved the efficient C-C coupling to form C2H6.

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