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The photocatalytic reduction of CO 2 to value-added methane (CH 4 ) has been a promising strategy for sustainable energy development, but it is challenging to trigger this reaction because of its necessary eight-electron transfer process. In this work, an efficient photocatalytic CO 2 -to-CH 4 reduction reaction was achieved for the first time in aqueous solution by using two crystalline heterogeneous catalysts, H{[Na 2 K 4 Mn 4 (PO 4 ) (H 2 O) 4 ]⊂{[Mo 6 O 12 (OH) 3 (HPO 4 ) 3 (PO 4 )] 4 [Mn 6 (H 2 O) 4 ]}·16H 2 O ( NENU-605 ) and H{[Na 6 CoMn 3 (PO 4 )(H 2 O) 4 ]⊂{[Mo 6 O 12 (OH) 3 (HPO 4 ) 3 (PO 4 )] 4 [Co 1.5 Mn 4.5 ]}·21H 2 O ( NENU-606 ). Both compounds have similar host inorganic polyoxometalate (POM) structures constructed with strong reductive {P 4 Mo 6  V } units, homo/hetero transition metal ions (Mn II /Co II Mn II ) and alkali metal ions (K + and/or Na + ). It is noted that the {P 4 Mo 6  V } cluster including the six Mo V atoms served as a multi-electron donor in the case of a photocatalytic reaction, while the transition metal ions functioned as catalytically active sites for adsorbing and activating CO 2 molecules. Additionally, the presence of alkali metal ions was believed to assist in the capture of more CO 2 for the photocatalytic reaction. The synergistic combination of the above-mentioned components in NENU-605 and NENU-606 effectively facilitates the accomplishment of the required eight-electron transfer process for CH 4 evolution. Furthermore, NENU-606 containing hetero-metallic active sites finally exhibited higher CH 4 generation selectivity (85.5%) than NENU-605 (76.6%).

chemical science

Hetero-metallic active sites coupled with strongly reductive polyoxometalate for selective photocatalytic CO<sub>2</sub>-to-CH<sub>4</sub> conversion in water

Hetero-metallic active sites coupled with strongly reductive polyoxometalate for selective photocatalytic CO2-to-CH4 conversion in water

Hetero-metallic active sites coupled with strongly reductive polyoxometalate for selective photocatalytic CO₂-to-CH₄ conversion in water