Issue 31, 2024

Dual-nodes bridged cobalt-modified Keggin-type polyoxometalate-based chains for highly efficient CO2 photoconversion

Abstract

The design of efficient catalysts for photocatalytic CO2 conversion is of great importance for the sustainable development of society. Herein, three polyoxometalate (POM)-based crystalline materials were formulated prepared by substituting transition metals and adjusting solvent acidity with 2-(2-pyridyl) benzimidazole (pyim) as the light-trapping ligand, namely {[SiW12O40][Co(pyim)2]2}·2C2H5OH (SiW12Co2), {[SiW12O40][Ni(pyim)2]2}·2C2H5OH (SiW12Ni2), and {[SiW12O40][Mn(pyim)2]2}·2C2H5OH (SiW12Mn2). X-ray crystallography diffraction analysis indicates that the three complexes exhibit isostructural properties, and form a stable one-dimensional chain structure stabilized by two [M(pyim)2]22+ (M = Co, Ni, and Mn) fragments serving as dual-nodes to the adjacent SiW12 units. A comprehensive analysis of the structural characterization and photocatalytic CO2 reduction properties is presented. Under light irradiation, SiW12Co2 exhibited a remarkable CO generation rate of 10 733 μmol g−1 h−1 with a turnover number of 328, outperforming most of the reported heterogeneous POM-based photocatalysts. Besides, cycling tests revealed that SiW12Co2 is an efficient and stable photocatalyst with great recyclability for at least four successive runs. This study proves that the successful incorporation of diverse transition metals into the POM anion could facilitate the development of highly efficient photocatalysts for the CO2RR.

Graphical abstract: Dual-nodes bridged cobalt-modified Keggin-type polyoxometalate-based chains for highly efficient CO2 photoconversion

Supplementary files

Article information

Article type
Paper
Submitted
17 Jun 2024
Accepted
11 Jul 2024
First published
16 Jul 2024

Dalton Trans., 2024,53, 12943-12950

Dual-nodes bridged cobalt-modified Keggin-type polyoxometalate-based chains for highly efficient CO2 photoconversion

X. Chen, J. Wu, J. Wang, X. Liu, H. Mei and Y. Xu, Dalton Trans., 2024, 53, 12943 DOI: 10.1039/D4DT01757A

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