Highly selective photoreduction of CO2 catalyzed by the encapsulated heterometallic-substituted polyoxometalate into a photo-responsive metal-organic framework

doi:10.1016/S1872-2067(23)64453-5

Abstract

Abstract:

The highly selective photoreduction of CO₂ into valuable chemical fuels such as CO has been considered as an effective strategy to address modern energy and environmental issues. In this work, we have adopted the well-established impregnation approach to construct a P₂W₁₅Ni₃{Re(CO)₃}₃@NU-1000 composite by incorporating heterometallic-substituted P₂W₁₅Ni₃{Re(CO)₃}₃ polyoxometalate (POM) into the pores of metal-organic framework (NU-1000) host. Upon light irradiation, the resulting P₂W₁₅Ni₃{Re(CO)₃}₃@NU-1000 composite can effectively photocatalyze CO₂ reduction, obtaining a CO production of 28982 μmol g^-1 with 93.5% selectivity during 10-h photocatalysis. The catalytic system exhibits great long-term recyclability and stability for at least four successive recycles. The proposed photocatalytic mechanism was confirmed by a series of photochemical and spectroscopic analyses.

Key words: CO₂ reduction, Polyoxometalate, Metal-organic framework, Heterometallic substitution, Photocatalysis

Huijie Li, Manzhou Chi, Xing Xin, Ruijie Wang, Tianfu Liu, Hongjin Lv, Guo-Yu Yang. Highly selective photoreduction of CO₂ catalyzed by the encapsulated heterometallic-substituted polyoxometalate into a photo-responsive metal-organic framework[J]. Chinese Journal of Catalysis, 2023, 50: 343-351.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64453-5

https://www.cjcatal.com/EN/Y2023/V50/I7/343

Figures/Tables 7

Scheme 1. Schematic illustration of the synthetic procedure of the P2W15Ni3{Re(CO)3}3@NU-1000 composite.

Fig. 1. SEM images of NU-1000 (a) and 1.13-P2W15Ni3 {Re(CO)3}3@NU-1000 composite (b). TEM images of NU-1000 (c) and 1.13-P2W15Ni3{Re(CO)3}3@NU-1000 composite (d). (e) selective SEM image and the corresponding elemental mapping images of 1.13-P2W15Ni3{Re(CO)3}3@NU-1000 composite.

Fig. 2. (a) The pore size distribution curves of P2W15Ni3{Re(CO)3}3, NU-1000, and P2W15Ni3{Re(CO)3}3@NU-1000; UV-vis diffuse reflectance spectra (b), FT-IR spectra (c), and PXRD patterns (d) of P2W15Ni3{Re(CO)3}3, NU-1000, and 1.13-P2W15Ni3{Re(CO)3}3@NU-1000 composite.

Fig. 3. (a) The yield of gas products in the photocatalytic CO2 reduction with different molar ratios of P2W15Ni3{Re(CO)3}3@NU-1000 in 10 h. (b) Control experiments of CO2 reduction by varying experimental conditions (Note: the moles of comparative catalysts including P2W15Ni3{Re(CO)3}3, NU-1000, Re(CO)5Cl, NiCl2, and others were kept the same as that in 1 mg 1.13-P2W15Ni3{Re(CO)3}3@NU-1000 photocatalyst). (c) Recycling tests of the 1.13-P2W15Ni3{Re(CO)3}3@NU-1000 photocatalyst. (d) Long-term photocatalytic CO2 reduction using 1.13-P2W15Ni3{Re(CO)3}3@NU-1000 composite.

Fig. 4. PL spectra (a) and normalized time-resolved PL decay kinetics (b) of NU-1000 and 1.13-P2W15Ni3{Re(CO)3}3@NU-1000 solid samples upon excitation at 365 nm.

Fig. 5. (a) High-resolution XPS spectra of Zr 3d in NU-1000 and 1.13-P2W15Ni3{Re(CO)3}3@NU-1000 before and after photocatalysis; high-resolution XPS spectra of Ni 2p (b), W 4f (c), and Re 4f (d) in 1.13-P2W15Ni3{Re(CO)3}3@NU-1000 before and after photocatalysis.

Fig. 6. Schematic diagram of the proposed photocatalytic CO2 reduction mechanism using P2W15Ni3{Re(CO)3}3@NU-1000 photocatalyst.

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Highly selective photoreduction of CO₂ catalyzed by the encapsulated heterometallic-substituted polyoxometalate into a photo-responsive metal-organic framework

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