Manipulating metal oxidation state over ultrastable metal-organic frameworks for boosting photocatalysis

Gong, Yun‐Nan; Mei, Jian-Hua; Liu, Jin-Wang; Huang, Hai‐Hua; Zhang, Jihong; Li, Xiaokang; Zhong, Di‐Chang; Lu, Tong‐Bu

doi:10.1016/j.apcatb.2021.120156

Cited by 66 publications

(14 citation statements)

References 78 publications

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“…As Ce-oxo clusters have been deemed as promising catalysts/supports for photocatalysis, ,− we investigated the photocatalytic oxidation of 4-methoxybenzyl alcohol (MBA) to 4-methoxybenzyl aldehyde (MBAD) to probe the clusters’ catalytic reactivities (Scheme ). We then utilized the newly synthesized Ce-oxo clusters as photocatalysts in toluene to determine their reactivity in both selectivity and yield.…”

Section: Resultsmentioning

confidence: 99%

Mechanistic Investigation of Enhanced Catalytic Selectivity toward Alcohol Oxidation with Ce Oxysulfate Clusters

et al. 2022

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Ceria-based materials have been highly desired in photocatalytic reactions due to their redox properties and strong oxygen storage and transfer ability. Herein, we report the structures of one CeCe 70 oxysulfate cluster and four MCe 70 clusters (M = Cu, Ni, Co, and Fe) with the same Ce 70 core. As noted, single-crystal X-ray diffraction confirmed the structures of CeCe 70 and the MCe 70 series, while Raman spectroscopy indicated an increase in oxygen defects upon the introduction of Cu and Fe ions. The clusters catalyzed the oxidation of 4-methoxybenzyl alcohol under ultraviolet light. CuCe 70 and FeCe 70 exhibited enhanced reactivity compared to CeCe 70 and improved aldehyde selectivity compared to control experiments. In comparison with their homogeneous congeners, the CeCe 70 /MCe 70 clusters altered the location of radical generation from the bulk solution to the clusters' surfaces. Mechanistic studies highlight the role of oxygen defects and specific transition metal introduction for efficient photocatalysis. The mechanistic pathway in this study provides insight into how to select or design a highly selective catalyst for photocatalysis.

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Section: Resultsmentioning

confidence: 99%

Mechanistic Investigation of Enhanced Catalytic Selectivity toward Alcohol Oxidation with Ce Oxysulfate Clusters

et al. 2022

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“…5 Since then, the number of studies using MOFs for the solar-driven HER increased significantly, reflecting the interest in the field. 6–9 From the point of view of application, however, it would be desirable to develop MOF-based materials as photocatalysts to promote the overall water splitting (OWS) under sunlight irradiation into H 2 and O 2 in the absence of sacrificial electron donors or noble metals. 10,11 In 2017, Huang, Liu and co-workers reported a seminal work using MIL-53(Al)–NH 2 in the presence of Ni( ii ) cations coordinated to the amino group of the terephthalate ligand as a co-catalyst to promote the photocatalytic OWS under UV-vis light irradiation.…”

Section: Introductionmentioning

confidence: 99%

Mixed-metal Zr/Ti MIL-173 porphyrinic metal–organic frameworks as efficient photocatalysts towards solar-driven overall water splitting

et al. 2022

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“…However, their photocatalytic activity is hampered due to their rare active sites and inherent high exciton binding energy [164,165]. MOFs, by virtue of the abundance of active site and semiconductor-like band structure, are considered as another nominator but suffer from spontaneous and fast exciton quench [166][167][168][169][170][171][172]. By combining dynamic covalent chemistry of COFs with coordination chemistry of MOFs, novel MOFs, COFs as well as MOF@COF hybrids have been developed in the applications of photodegradation of pollutants, hydrogen generation, and organic transformation reactions [28,76,77,133,173].…”

Section: Photocatalysismentioning

confidence: 99%

Combining metal-organic frameworks (MOFs) and covalent-organic frameworks (COFs): Emerging opportunities for new materials and applications

Guo

Wan

et al. 2021

Nano Res.

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In the past decades, metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) basically enjoy the coordination chemistry and covalent chemistry, respectively, and such uniqueness has become the major obstacle hampering their further scope diversity and application multi-functionalization. Inspired from the principle of organic retrosynthesis, combining coordination bond and covalent bond together offers additional opportunities for constructing novel MOFs, COFs and MOF@COF hybrids as well as confer on them superior performances in versatile application fields. In this review, we firstly classify and summarize the recently reported synthesis strategies based on the integration of metal-ligand coordination and dynamic covalent bonds. Then, the application performances of as-constructed MOFs, COFs as well as MOF@COF hybrids are discussed and highlighted in the fields of adsorption, separation, catalysis, biosensing, energy storage and so on. Last, our personal insights of the remaining challenges and further prospects are also provided, in order to trigger much more inspirations and endeavors for this hot research field.

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Manipulating metal oxidation state over ultrastable metal-organic frameworks for boosting photocatalysis

Cited by 66 publications

References 78 publications

Mechanistic Investigation of Enhanced Catalytic Selectivity toward Alcohol Oxidation with Ce Oxysulfate Clusters

Mechanistic Investigation of Enhanced Catalytic Selectivity toward Alcohol Oxidation with Ce Oxysulfate Clusters

Mixed-metal Zr/Ti MIL-173 porphyrinic metal–organic frameworks as efficient photocatalysts towards solar-driven overall water splitting

Combining metal-organic frameworks (MOFs) and covalent-organic frameworks (COFs): Emerging opportunities for new materials and applications

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