Research on the Construction of a Series of Transition Metal-Substituted Keggin-Type TMSPOMs@PCN-224 Composites through the Encapsulation Method and Their Electron Transfer Mechanism in CO<sub>2</sub>RR

Zhang, Yan; Li, Can; Shu, Lei; Teng, Yun-Lei; Dong, Bao-Xia

doi:10.1021/acs.inorgchem.4c00840

Inorg. Chem.

2024

DOI: 10.1021/acs.inorgchem.4c00840

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Research on the Construction of a Series of Transition Metal-Substituted Keggin-Type TMSPOMs@PCN-224 Composites through the Encapsulation Method and Their Electron Transfer Mechanism in CO₂RR

Yan Zhang,

Can Li,

Lei Shu

et al.

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Cited by 2 publications

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Heterogenization of a Sandwich [(PW₉O₃₄)₂Co₄(H₂O)₂]¹⁰⁻ in PCN‐222/PCN‐222(M): Exploring the Electron Transfer for Electrocatalytic CO₂ Reduction

Shu,

Li,

Peng

et al. 2024

Eur J Inorg Chem

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In this study, we designed and prepared polyoxometalate@metal‐organic framework (POM@MOF) composite catalysts through the anchoring of a sandwich POM [(PW9O34)2Co4(H2O)2]10− (shortened as P2W18Co4) to the hexagonal channel of the PCN–222 (metal‐free) or PCN–222(M) (M=Fe, Co) frameworks. The composite materials were applied to the electrocatalytic reduction of CO2 reaction (CO2RR) to analyse the effect of incorporating P2W18Co4 on catalytic activity. The P2W18Co4@PCN–222 composite exhibited enhanced activity across a wide potential range (–0.60~ –0.85 V vs. RHE) and an optimal FECO of 72% at –0.75 V vs. RHE, which was more than double that of PCN–222 (FECO= 33%). The current density surpassed that of the PCN–222 precursors by over sixteen times at the same potential. In contrast, the P2W18Co4@PCN–222(M) composite demonstrated decreased current density, minimal enhancement in CO2RR activity, and a competing HER behaviour. Density functional theory calculations were conducted on simplified models of P2W18Co4@H2–TCPP and P2W18Co4@M–TCPP to elucidate the divergent catalytic performances. The findings revealed that while both configurations exhibited the same rate‐limiting step (formation of the *COOH intermediate), a significantly reduced reaction barrier was only observed in the P2W18Co4@H2–TCPP setup, explaining its substantial activity improvement.

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Heterogenization of a Sandwich [(PW₉O₃₄)₂Co₄(H₂O)₂]¹⁰⁻ in PCN‐222/PCN‐222(M): Exploring the Electron Transfer for Electrocatalytic CO₂ Reduction

Shu,

Li,

Peng

et al. 2024

Eur J Inorg Chem

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Incorporation of a Binuclear Cobalt Complex into MOFs for Photocatalytic CO₂ Reduction with H₂O as an Electron Donor

Wang,

Yuan,

Feng

et al. 2024

Inorg. Chem.

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The development of molecular composite photocatalysts for costeffective, sacrificial-reagent-free CO 2 reduction is desirable but challenging. Herein, we employed an in situ encapsulation strategy to encapsulate the binuclear cobalt complex (Co 2 L) within NH 2 -MIL-125 and synthesized a range of MOF-based composites with varying cobalt content for photocatalytic CO 2 reduction. The photocatalytic results showed that the catalytic performance increased with the increase in Co 2 L content, reaching a rapid CO generation rate of 27.95 μmol•g −1 • h −1 , over 5 times that of bare NH 2 -MIL-125, with water as the electron donor instead of any organic sacrificial agent. This composite catalyst effectively harnesses the advantages of both molecular catalysts and MOFs, leveraging the superior catalytic activity of molecular catalysts while also capitalizing on the light absorption and water oxidation capabilities of MOFs, resulting in a remarkable ability for photocatalytic CO 2 reduction. The photocatalytic mechanism involving electron transfer and CO 2 activation has been revealed by photoluminescence spectroscopy, in situ X-ray photoelectron spectroscopy, in situ diffuse reflectance infrared Fourier transform spectroscopy, and other control experiments.

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Research on the Construction of a Series of Transition Metal-Substituted Keggin-Type TMSPOMs@PCN-224 Composites through the Encapsulation Method and Their Electron Transfer Mechanism in CO₂RR

Cited by 2 publications

References 55 publications

Heterogenization of a Sandwich [(PW₉O₃₄)₂Co₄(H₂O)₂]¹⁰⁻ in PCN‐222/PCN‐222(M): Exploring the Electron Transfer for Electrocatalytic CO₂ Reduction

Heterogenization of a Sandwich [(PW₉O₃₄)₂Co₄(H₂O)₂]¹⁰⁻ in PCN‐222/PCN‐222(M): Exploring the Electron Transfer for Electrocatalytic CO₂ Reduction

Incorporation of a Binuclear Cobalt Complex into MOFs for Photocatalytic CO₂ Reduction with H₂O as an Electron Donor

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Research on the Construction of a Series of Transition Metal-Substituted Keggin-Type TMSPOMs@PCN-224 Composites through the Encapsulation Method and Their Electron Transfer Mechanism in CO2RR

Cited by 2 publications

References 55 publications

Heterogenization of a Sandwich [(PW9O34)2Co4(H2O)2]10− in PCN‐222/PCN‐222(M): Exploring the Electron Transfer for Electrocatalytic CO2 Reduction

Heterogenization of a Sandwich [(PW9O34)2Co4(H2O)2]10− in PCN‐222/PCN‐222(M): Exploring the Electron Transfer for Electrocatalytic CO2 Reduction

Incorporation of a Binuclear Cobalt Complex into MOFs for Photocatalytic CO2 Reduction with H2O as an Electron Donor

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Product

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Research on the Construction of a Series of Transition Metal-Substituted Keggin-Type TMSPOMs@PCN-224 Composites through the Encapsulation Method and Their Electron Transfer Mechanism in CO₂RR

Heterogenization of a Sandwich [(PW₉O₃₄)₂Co₄(H₂O)₂]¹⁰⁻ in PCN‐222/PCN‐222(M): Exploring the Electron Transfer for Electrocatalytic CO₂ Reduction

Heterogenization of a Sandwich [(PW₉O₃₄)₂Co₄(H₂O)₂]¹⁰⁻ in PCN‐222/PCN‐222(M): Exploring the Electron Transfer for Electrocatalytic CO₂ Reduction

Incorporation of a Binuclear Cobalt Complex into MOFs for Photocatalytic CO₂ Reduction with H₂O as an Electron Donor