Uranyl photocatalysis: precisely controlled oxidation of sulfides with ground-state oxygen

He, Wei; Lin, Ying Wu; Yu, Donghong

doi:10.1007/s11426-019-9675-5

Cited by 17 publications

(13 citation statements)

References 4 publications

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“…Meanwhile, most of sulfones have a wide range of biological activities (showing good effects in insecticide, bactericidal, antiviral, and other drugs) and have been widely used in pesticides, medicine, and other fields . However, there are still some problems hindering the development of the oxidation of thioethers, including high-temperature reaction requirement, ,, the selectivity of products (sulfoxide and sulfone), − the stability of catalysts, etc. Therefore, the solution to overcome a series of problems is to design and explore a kind of mild, highly selective, and stable catalyst.…”

Section: Resultsmentioning

confidence: 99%

ZnO–POM Cluster Sub-1 nm Nanosheets as Robust Catalysts for the Oxidation of Thioethers at Room Temperature

2021

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Two-dimensional (2D) zinc oxides have attracted more and more research interests due to their unique properties. Yet, it remains a great challenge to limit the thickness to the sub-1 nm scale and further combine with other components to obtain 2D hybrid zinc oxide (ZnO)-based sub-1 nm materials. Herein, a versatile strategy was successfully developed to realize the controllable preparation of ZnO–polyoxometalate (POM)-based 2D hybrid sub-1 nm nanosheet (HSNS) superstructures by incorporating three kinds of molybdenum-based POM clusters into the zinc oxide system. Molecular dynamics simulation results demonstrated that POM clusters interact with ZnO/Zn(OH)2 molecules and coassembled into stable 2D HSNSs. Significantly, theses materials as robust catalysts showed excellent catalytic activity, selectivity, and stability in the oxidation of thioethers at room temperature, which partly can be attributed to the special 2D sub-1 nm nanostructures with large specific areas leading to the full exposure of active sites. Meanwhile, the synergetic effect of multiple components also played an important role during the catalytic process. Thus, this work would pave the way for the precise synthesis of multicomponent 2D hybrid sub-1 nm materials for widespread applications.

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Section: Resultsmentioning

confidence: 99%

ZnO–POM Cluster Sub-1 nm Nanosheets as Robust Catalysts for the Oxidation of Thioethers at Room Temperature

2021

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“…With excellent photocatalytic properties of uranyl ions [88], uranyl photocleavage has been observed not only for DNA/RNA [75,89], but also proteins, especially for those with phosphorylation, such as α-/β-casein and ovalbumin [90]. Duff and Kumar first demonstrated that UO 2 2+ was able to cleave a number of proteins, including BSA, HSA, porcine SA (PSA), glucose oxidase and transferrin, as induced by visible light irradiation (420-460 nm) [91].…”

Section: Protein/dna Cleavage and Other Impactsmentioning

confidence: 99%

Uranyl Binding to Proteins and Structural-Functional Impacts

Lin

2020

Biomolecules

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The widespread use of uranium for civilian purposes causes a worldwide concern of its threat to human health due to the long-lived radioactivity of uranium and the high toxicity of uranyl ion (UO 2 2+ ). Although uranyl-protein/DNA interactions have been known for decades, fewer advances are made in understanding their structural-functional impacts. Instead of focusing only on the structural information, this article aims to review the recent advances in understanding the binding of uranyl to proteins in either potential, native, or artificial metal-binding sites, and the structural-functional impacts of uranyl-protein interactions, such as inducing conformational changes and disrupting protein-protein/DNA/ligand interactions. Photo-induced protein/DNA cleavages, as well as other impacts, are also highlighted. These advances shed light on the structure-function relationship of proteins, especially for metalloproteins, as impacted by uranyl-protein interactions. It is desired to seek approaches for biological remediation of uranyl ions, and ultimately make a full use of the double-edged sword of uranium.Proteins, especially for metalloproteins, play vital roles in supporting life, including electron-transfer, O 2 -binding and delivery, and catalysis, etc [11][12][13][14][15][16][17][18]. To date, a plenitude of proteins have been shown to interact with UO 2 2+ , such as proteins in blood (human serum albumin, HSA; transferrin, Tf;hemoglobin, Hb), proteins involved in bone growth (osteopontin, OPN; fetuin-A), and the intracellar proteins (metallothionein, MT; cytochromes b 5 /c; Cyt b 5 /c; calmodulin, CaM), etc [19]. Although the structural features of some uranyl-protein complexes are well-documented [7-9], fewer advances are made in understanding the functional impacts of uranyl-protein interactions, with much less for other actinides-proteins interactions, as reviewed by Creff et al. very recently [20]. Instead of focusing only on the structural information, this review highlights the recent advances in understanding the binding of uranyl to proteins, as illustrated in Scheme 1, in either potential, native or artificial metal-binding sites, or the corresponding structural-functional impacts, such as inducing conformational changes and disrupting protein-protein/DNA/ligand interactions. Future directions for studying uranyl-protein interactions are also prospected.

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“…Sulfide oxidation has attracted long standing interest, both in industry and the academic world, because the final products, sulfoxides and sulfones, are important intermediates for the preparation of chemically and biologically significant molecules. [1][2][3][4] For the oxidation of sulfides to sulfoxides/ sulfones, H 2 O 2 occupies a predominant position, as it is inexpensive, non-toxic, and forms water as the sole byproduct. [5][6][7][8][9] Nevertheless, in the absence of catalyst, the oxidation process employing H 2 O 2 is very slow.…”

Section: Introductionmentioning

confidence: 99%

“…[17][18][19][20] Phosphonate acids were frequently applied as bridging ligands by many of these titanium oxo-clusters, demonstrating their strong coordination ability for titanium oxo-clusters. Apart from the titanium oxoclusters coordinated by small ligands, the titanium oxo-clusters coordinated by macrocyclic ligands, such as calkylpyrogallol [4]arenes, [21] p-tert-butylcalix [n]arene (H n CnA, n = 4, 6, 8), [22][23][24] and p-tert-butylthiacalix [4]arene (H 4 TC4A), [25,26] also received some attention recently due to their attractive architectural beauty and immense technological applications. Among them, calix[n]arene with abundant tertiary butyl and phenol groups is an effective bridging and protecting ligand for complexes.…”

Section: Introductionmentioning

confidence: 99%

Solvent‐Polarity‐Induced Assembly of Calixarene‐Capped Titanium‐Oxo Clusters with Catalytic Activity in the Oxygenation of Sulfides

et al. 2022

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Four calixarene-coordinated titanium-oxo clusters, namely, [Ti 4 (C6A) 2 (μ 3 -O) 2 (DMF) 2 ] (CIAC-258), [Ti 8 (H 3 C6A) 4 (C 6 H 5 PO 3 ) 8 (μ 2 -O) 4 ] 4À (CIAC-259), [Ti 6 (TC4A) 3 (μ 2 -O) 3 (OiPr) 6 ] (CIAC-260) and [Ti 6 (H 2 TC4A) 4 (C 6 H 5 PO 3 ) 4 (μ 2 -O) 5 (DMF) 2 ] 2À (CIAC-261) were obtained, which feature sandwich-like, windmill-like, triangular, and tetrahedral structures, respectively. The polarity of the solvent determines the involvement of the auxiliary ligand phenylphosphonic acid in the formation of the products and their structures. Compounds CIAC-258 and CIAC-261 exhibit good catalytic performance in the selective oxidation of sulfides to sulfoxides with H 2 O 2 as the oxidant, which can be attributed to the Ti active sites coordinated by exchangeable DMF molecules. Moreover, density functional theory (DFT) calculations revealed that the Ti-hydroperoxo species formed by the interaction of the Ti active site in CIAC-258 or CIAC-261 and H 2 O 2 is the most likely catalytic active component during the catalytic sulfoxidation process.

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Uranyl photocatalysis: precisely controlled oxidation of sulfides with ground-state oxygen

Cited by 17 publications

References 4 publications

ZnO–POM Cluster Sub-1 nm Nanosheets as Robust Catalysts for the Oxidation of Thioethers at Room Temperature

ZnO–POM Cluster Sub-1 nm Nanosheets as Robust Catalysts for the Oxidation of Thioethers at Room Temperature

Uranyl Binding to Proteins and Structural-Functional Impacts

Solvent‐Polarity‐Induced Assembly of Calixarene‐Capped Titanium‐Oxo Clusters with Catalytic Activity in the Oxygenation of Sulfides

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