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Photocatalytic CO 2 reduction into energy carriers is of utmost importance due to the rising concentrations of CO 2 and the depleting energy resource. However, the highly selective generation of desirable hydrocarbon fuel, such as methane (CH 4 ), from CO 2 remains extremely challenging. Herein, we present two stable polyoxometalate-grafted metalloporphyrin coordination frameworks (POMCFs), which are constructed with reductive Zn-ϵ-Keggin clusters and photosensitive tetrakis(4-carboxylphenyl)porphyrin (H 2 TCPP) linkers, exhibiting high selectivity (&gt;96%) for CH 4 formation in a photocatalytic CO 2 -reduction system. To our knowledge, the high CH 4 selectivity of POMCFs has surpassed all of the reported coordination-framework-based heterogeneous photocatalysts for CO 2 -to-CH 4 conversion. Significantly, the introduction of a Zn-ϵ-keggin cluster with strong reducing ability is the important origin for POMCFs to obtain high photocatalytic selectivity for CH 4 formation, considering that eight Mo V atoms can theoretically donate eight electrons to fulfill the multielectron reduction process of CO 2 -to-CH 4 transformation.

Multielectron transportation of polyoxometalate-grafted metalloporphyrin coordination frameworks for selective CO2-to-CH4 photoconversion