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Nuclearity enlargement from [PW₉O₃₄@Ag₅₁] to [(PW₉O₃₄)₂@Ag₇₂] and 2D and 3D network formation driven by bipyridines.

ABSTRACT: The structural transformations of metal nanoclusters are typically quite complex processes involving the formation and breakage of several bonds, and thus are challenging to study. Herein, we report a case where two lacunary Keggin polyoxometallate templated silver single-pods [PW₉O₃₄@Ag₅₁] (SD/Ag51b) fuse to a double-pod [(PW₉O₃₄)₂@Ag₇₂] by reacting with 4,4'-bipyridine (bipy) or 1,4-bis(4-pyridinylmethyl)piperazine (pi-bipy). Their crystal structures reveal the formation of a 2D 4⁴-sql layer (SD/Ag72a) with bipy and a 3D pcu framework (SD/Ag72c) with pi-bipy. The PW₉O₃₄^9- retains its structure during the cluster fusion and cluster-based network formation. Although the two processes, stripping of an Ag-ligands interface followed by fusion, and polymerization, are difficult to envisage, electrospray ionization mass spectrometry provides enough evidences for such a proposal to be made. Through this example, we expect the structural transformation to become a powerful method for synthesizing silver nanoclusters and their infinite networks, and to evolve from trial-and-error to rational.

SUBMITTER: Wang Z

PROVIDER: S-EPMC8979969 | biostudies-literature | 2022 Apr

REPOSITORIES: biostudies-literature

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Nuclearity enlargement from [PW9O34@Ag51] to [(PW9O34)2@Ag72] and 2D and 3D network formation driven by bipyridines.

Wang Zhi Z Zhu Yan-Jie YJ Li Ying-Zhou YZ Zhuang Gui-Lin GL Song Ke-Peng KP Gao Zhi-Yong ZY Dou Jian-Min JM Kurmoo Mohamedally M Tung Chen-Ho CH Sun Di D

Nature communications 20220404 1

The structural transformations of metal nanoclusters are typically quite complex processes involving the formation and breakage of several bonds, and thus are challenging to study. Herein, we report a case where two lacunary Keggin polyoxometallate templated silver single-pods [PW9O34@Ag51] (SD/Ag51b) fuse to a double-pod [(PW9O34)2@Ag72] by reacting with 4,4'-bipyridine (bipy) or 1,4-bis(4-pyridinylmethyl)piperazine (p ...[more]

PMID: 35379821

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Project description:Photocatalyst is the core of photocatalysis and directly determines photocatalytic performance. However, low quantum efficiency and low utilization of solar energy are important technical problems in the application of photocatalysis. In this work, a series of polyoxometalates (POMs) [H3PW12O40] (PW12)-doped titanium dioxide (TiO2) nanofibers modified with various amount of silver (Ag) nanoparticles (NPs) were prepared by utilizing electrospinning/photoreduction strategy, and were labelled as x wt% Ag/PW12/TiO2 (abbr. x% Ag/PT, x = 5, 10, and 15, respectively). The as-prepared materials were characterized with a series of techniques and exhibited remarkable catalytic activities for visible-light degradation tetracycline (TC), enrofloxacin (ENR), and methyl orange (MO). Particularly, the 10% Ag/PT catalyst with a specific surface area of 155.09 m2/g and an average aperture of 4.61 nm possessed the optimal photodegradation performance, with efficiencies reaching 78.19% for TC, 93.65% for ENR, and 99.29% for MO, which were significantly higher than those of PW12-free Ag/TiO2 and PT nanofibers. Additionally, various parameters (the pH of the solution, catalyst usage, and TC concentration) influencing the degradation process were investigated in detail. The optimal conditions are as follows: catalyst usage: 20 mg; TC: 20 mL of 20 ppm; pH = 7. Furthermore, the photodegradation intermediates and pathways were demonstrated by HPLC-MS measurement. We also investigated the toxicity of products generated during TC removal by employing quantitative structure-activity relationship (QSAR) prediction through a toxicity estimation software tool (T.E.S.T. Version 5.1.2.). The mechanism study showed that the doping of PW12 and the modification of Ag NPs on TiO2 broadened the visible-light absorption, accelerating the effective separation of photogenerated carriers, therefore resulting in an enhanced photocatalytic performance. The research provided some new thoughts for exploiting efficient and durable photocatalysts for environmental remediation.

Dataset Information

Nuclearity enlargement from [PW₉O₃₄@Ag₅₁] to [(PW₉O₃₄)₂@Ag₇₂] and 2D and 3D network formation driven by bipyridines.

Publications

Nuclearity enlargement from [PW<sub>9</sub>O<sub>34</sub>@Ag<sub>51</sub>] to [(PW<sub>9</sub>O<sub>34</sub>)<sub>2</sub>@Ag<sub>72</sub>] and 2D and 3D network formation driven by bipyridines.

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