A benzothiadiazole-based Pt(<scp>ii</scp>) coordination polymer as an efficient heterogeneous photocatalyst for visible-light-driven aerobic oxidative coupling of amines

Ahmed, Shakil; Kumar, Atul; Mukherjee, Partha Sarathi

doi:10.1039/d3cc00021d

Cited by 11 publications

(6 citation statements)

References 27 publications

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“…Benzylamine coupling has been widely reported as one of the common photocatalytic oxidation reactions, and molecular oxygen is generally involved in this reaction in the form of superoxide radicals [47–50] . It should be mentioned that 1 O 2 ‐driven benzylamine coupling oxidation reactions have also been reported [51–53] . As discussed above, PCC‐6‐Ni favors the production of superoxide radicals while PCC‐6‐Zn promotes the generation of singlet oxygen.…”

Section: Resultsmentioning

confidence: 94%

“…[47][48][49][50] It should be mentioned that 1 O 2 -driven benzylamine coupling oxidation reactions have also been reported. [51][52][53] As discussed above, PCC-6-Ni favors the production of superoxide radicals while PCC-6-Zn promotes the generation of singlet oxygen. Thus, we the photocatalytic properties of PCC-6-M by a transformation of benzylamine to N-(phenylmethylene)benzenemethanamine.…”

Section: Methodsmentioning

confidence: 91%

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Modeling the Enzyme Specificity by Molecular Cages through Regulating Reactive Oxygen Species Evolution

et al. 2023

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Mimicking the active site and the substrate binding cavity of the enzyme to achieve specificity in catalytic reactions is an essential challenge. Herein, porous coordination cages (PCCs) with intrinsic cavities and tunable metal centers have proved the regulation of reactive oxygen species (ROS) generating pathways as evidenced by multiple photo-induced oxidations. Remarkably, in the presence of the Zn 4 -μ 4 -O center, PCC converted dioxygen molecules from triplet to singlet excitons, whereas the Ni 4 -μ 4 -O center promoted the efficient dissociation of electrons and holes to conduct electron transfer towards substrates. Accordingly, the distinct ROS generation behavior of PCC-6-Zn and PCC-6-Ni enables the conversion of O 2 to 1 O 2 and O 2 *À , respectively. In contrast, the Co 4 -μ 4 -O center combined the 1 O 2 and O 2 *Àtogether to generate carbonyl radicals, which in turn reacted with the oxygen molecules. Harnessing the three oxygen activation pathways, PCC-6-M (M = Zn/Ni/Co) display specific catalytic activities in thioanisole oxidation (PCC-6-Zn), benzylamine coupling (PCC-6-Ni), and aldehyde autoxidation (PCC-6-Co). This work not only provides fundamental insights into the regulation of ROS generation by a supramolecular catalyst but also demonstrates a rare example of achieving reaction specificity through mimicking natural enzymes by PCCs.

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Section: Resultsmentioning

confidence: 94%

Section: Methodsmentioning

confidence: 91%

Modeling the Enzyme Specificity by Molecular Cages through Regulating Reactive Oxygen Species Evolution

et al. 2023

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“…[47][48][49][50] It should be mentioned that 1 O 2 -driven benzylamine coupling oxidation reactions have also been reported. [51][52][53] As discussed above, PCC-6-Ni favors the production of superoxide radicals while PCC-6promotes the generation of singlet oxygen. Thus, we explored the photocatalytic properties of PCC-6-M by a transformation of benzylamine to N-(phenylmethylene)benzenemethanamine.…”

Section: Co Respectively According To the Equation Of Ementioning

confidence: 91%

Modeling the Enzyme Specificity by Molecular Cages through Regulating Reactive Oxygen Species Evolution

et al. 2023

View full text Add to dashboard Cite

Mimicking the active site and the substrate binding cavity of the enzyme to achieve specificity in catalytic reactions is an essential challenge. Herein, porous coordination cages (PCCs) with intrinsic cavities and tunable metal centers have proved the regulation of reactive oxygen species (ROS) generating pathways as evidenced by multiple photo‐induced oxidations. Remarkably, in the presence of the Zn4‐μ4‐O center, PCC converted dioxygen molecules from triplet to singlet excitons, whereas the Ni4‐μ4‐O center promoted the efficient dissociation of electrons and holes to conduct electron transfer towards substrates. Accordingly, the distinct ROS generation behavior of PCC‐6‐Zn and PCC‐6‐Ni enables the conversion of O2 to 1O2 and O2⋅−, respectively. In contrast, the Co4‐μ4‐O center combined the 1O2 and O2⋅− together to generate carbonyl radicals, which in turn reacted with the oxygen molecules. Harnessing the three oxygen activation pathways, PCC‐6‐M (M=Zn/Ni/Co) display specific catalytic activities in thioanisole oxidation (PCC‐6‐Zn), benzylamine coupling (PCC‐6‐Ni), and aldehyde autoxidation (PCC‐6‐Co). This work not only provides fundamental insights into the regulation of ROS generation by a supramolecular catalyst but also demonstrates a rare example of achieving reaction specificity through mimicking natural enzymes by PCCs.

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“…Considerable interest has aroused for hybrid MPCs because of their wide variety of biomedical and industrial applications. ,, Furthermore, MPCs are one of the most useful systems in bio separation, magnetic resonance imaging, cancer treatment, drug delivery, and antimalarial activity . The hybrid structures of polymers and metals can be found in the vehicle industry as anti-knocking components , and also as photocatalysts in the treatment of organic dyes in wastewater. − …”

Section: Introductionmentioning

confidence: 99%

Photocatalytic Activity and Thermal Stability of Hybrid Metal–Polymer-Coordinated Complexes Derived from Gallic Acid and Ethylenediamine

Kayed

Almeataq

2023

Langmuir

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Three new hybrid metal–polymer-coordinated complexes (MPCs) of copper(II), cobalt(II), and nickel(II) ions with an organic polymer derived from gallic acid and ethylenediamine (GAEtH) were synthesized. The structures of GAEtH and MPCs were characterized with FT-IR, ultraviolet (UV)–Vis, 1H and 13C NMR spectroscopy, and elemental and thermogravimetric analysis. The results reveal that the organic polymer GAEtH exhibits an infinite one-dimensional chain structure, while the hybrid MPCs have a double chain structure, with the two chains joined by metal ions. The thermodynamic and kinetic parameters of the thermal degradation stages were determined by the Coats Redfern method, and the photocatalytic behaviors of the MPCs were investigated through the decomposition of methyl orange dye under UV irradiation.

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A benzothiadiazole-based Pt(ii) coordination polymer as an efficient heterogeneous photocatalyst for visible-light-driven aerobic oxidative coupling of amines

Abstract: An emissive Pt(II) coordination polymer (TBP) was synthesized by assembling a benzothiadiazole-based Pt(II) acceptor (A) with tetraphenylethene (TPE) containing donor (L). Multiple benzothiadiazole units in the polymeric array of the...

Cited by 11 publications

References 27 publications

Modeling the Enzyme Specificity by Molecular Cages through Regulating Reactive Oxygen Species Evolution

Modeling the Enzyme Specificity by Molecular Cages through Regulating Reactive Oxygen Species Evolution

Modeling the Enzyme Specificity by Molecular Cages through Regulating Reactive Oxygen Species Evolution

Photocatalytic Activity and Thermal Stability of Hybrid Metal–Polymer-Coordinated Complexes Derived from Gallic Acid and Ethylenediamine

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