Iridium complex modified MOFs for enhancing photocatalytic hydrogen evolution

Wang, Yue; Huang, Yifan; Liu, Shihan; Cui, Shuaichuan; Zhang, Yifan; Deng, Pengyang

doi:10.1039/d4ya00184b

Energy Adv.

2024

DOI: 10.1039/d4ya00184b

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Iridium complex modified MOFs for enhancing photocatalytic hydrogen evolution

Yue Wang,

Yifan Huang,

Shihan Liu

et al.

Abstract: In this paper, we prepared an iridium(III) complex modified MOF (cmrIr/Pt@UiO-66-NH2) to combine the excellent light absorption properties of iridium(III) complexes and good photostability of metal-organic frameworks (MOF). Photocatalytic tests...

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Efficient Ir^III Photosensitizer Incorporated in the Metal–Organic Framework with the Bis-lophine-bipyridine Motif for C(sp³)-C/N–H Cross-Coupling Reactions

Chen,

Liu,

Chen

et al. 2024

ACS Catal.

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Photocatalytic technology offers a potential solution to energy and environmental issues. The performance of photocatalysts directly affects the efficiency of photocatalysis. Iridium(III)-based catalysts have garnered attention due to their unique electronic structure and high catalytic activity. However, most Ir III catalysts are homogeneous and face issues such as low stability and difficulty in recycling. The research on heterogeneous Ir III catalysts has become a hot topic, aiming to improve their stability and recyclability. In this study, we designed a tetracarboxylate ligand containing bipyridine modified with a bilophthalene unit, constructed a Zr-based metal−organic framework (MOF) with a 2-fold interpenetrating structure, and introduced [Ir III (ppy) 2 ] + units through postmodification to form Ir@Zr-MOF. The heterostructure enhanced the utilization of light energy and photocatalytic efficiency. Apart from the electron transfer pathway between the original zirconium clusters and the bislophine-bipyridine unit, comparative studies of theoretical models showed that the introduction of the [Ir III (ppy) 2 ] + unit reduced the energy level and enhanced the absorption of visible light in the 500−550 nm range, corresponding to the charge transfer between the modified bis-lophine-bipyridine and [Ir III (ppy) 2 ] + unit. Ir@Zr-MOF, as a photocatalyst, can facilitate the trifluoromethylation of coumarins and the oxidative dehydrogenative coupling reaction of ethers with aryl hydrazones. The conversion yields of the related reactions can reach up to 95%. The mechanism presumes that the generation of superoxide radicals and the corresponding holes produced by Ir@Zr-MOF are crucial for the photocatalytic reaction. The generation of superoxide radicals can be verified by ESR. The host−guest interactions and hole effects of Ir@Zr-MOF with reaction substrates were also explored through theoretical simulations. This work provides a strategy for the heterogenization of Ir III catalysts, offering insights for the preparation of photosensitizers and the enhancement of light energy utilization.

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Efficient Ir^III Photosensitizer Incorporated in the Metal–Organic Framework with the Bis-lophine-bipyridine Motif for C(sp³)-C/N–H Cross-Coupling Reactions

Chen,

Liu,

Chen

et al. 2024

ACS Catal.

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Iridium complex modified MOFs for enhancing photocatalytic hydrogen evolution

Abstract: In this paper, we prepared an iridium(III) complex modified MOF (cmrIr/Pt@UiO-66-NH2) to combine the excellent light absorption properties of iridium(III) complexes and good photostability of metal-organic frameworks (MOF). Photocatalytic tests...

Cited by 1 publication

References 47 publications

Efficient Ir^III Photosensitizer Incorporated in the Metal–Organic Framework with the Bis-lophine-bipyridine Motif for C(sp³)-C/N–H Cross-Coupling Reactions

Efficient Ir^III Photosensitizer Incorporated in the Metal–Organic Framework with the Bis-lophine-bipyridine Motif for C(sp³)-C/N–H Cross-Coupling Reactions

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Iridium complex modified MOFs for enhancing photocatalytic hydrogen evolution

Abstract: In this paper, we prepared an iridium(III) complex modified MOF (cmrIr/Pt@UiO-66-NH2) to combine the excellent light absorption properties of iridium(III) complexes and good photostability of metal-organic frameworks (MOF). Photocatalytic tests...

Cited by 1 publication

References 47 publications

Efficient IrIII Photosensitizer Incorporated in the Metal–Organic Framework with the Bis-lophine-bipyridine Motif for C(sp3)-C/N–H Cross-Coupling Reactions

Efficient IrIII Photosensitizer Incorporated in the Metal–Organic Framework with the Bis-lophine-bipyridine Motif for C(sp3)-C/N–H Cross-Coupling Reactions

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Product

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About

Efficient Ir^III Photosensitizer Incorporated in the Metal–Organic Framework with the Bis-lophine-bipyridine Motif for C(sp³)-C/N–H Cross-Coupling Reactions

Efficient Ir^III Photosensitizer Incorporated in the Metal–Organic Framework with the Bis-lophine-bipyridine Motif for C(sp³)-C/N–H Cross-Coupling Reactions