Demystifying the roles of single metal site and cluster in CO2 reduction via light and electric dual-responsive polyoxometalate-based metal-organic frameworks

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Abstract

Photo- or electroreduction of carbon dioxide into highly valued products offers a promising strategy to achieve carbon neutrality. Here, a series of polyoxometalate-based metal-organic frameworks (M-POMOFs) were constructed by metalloporphyrins [tetrakis(4-carboxyphenyl)-porphyrin-M (M-TCPPs)] and reductive POM for photo- and electrocatalytic carbon dioxide reductions (PCR and ECR, respectively), and the mysteries between the roles of single metal site and cluster in catalysis were disclosed. Iron-POMOF exhibited an excellent selectivity (97.2%) with high methane production of 922 micromoles per gram in PCR, together with superior Faradaic efficiency for carbon dioxide to carbon monoxide (92.1%) in ECR. The underlying mechanisms were further clarified. Photogenerated electrons transferred from iron-TCPP to the POM cluster for methane generation under irradiation, while the abundant electrons flowed to the center of iron-TCPP for carbon monoxide formation under the applied electric field. The specific multielectron products generated on iron-POMOF through switching driving forces to control electron flow direction between single metal site and cluster catalysis.

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Huang, Q., Niu, Q., Li, X. F., Liu, J., Sun, S. N., Dong, L. Z., … Lan, Y. Q. (2022). Demystifying the roles of single metal site and cluster in CO2 reduction via light and electric dual-responsive polyoxometalate-based metal-organic frameworks. Science Advances, 8(49). https://doi.org/10.1126/sciadv.add5598

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