Self-assembly of polyoxometalate clusters into two-dimensional clusterphene structures featuring hexagonal pores

Liu, Qingda; Zhang, Qinghua; Shi, Wenxiong; Hu, Han‐Shi; Zhuang, Jing; Wang, Xun

doi:10.1038/s41557-022-00889-1

Cited by 93 publications

(63 citation statements)

References 26 publications

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“…Thus, POM-based SNMs show high potential for TEO reaction catalysis. 70 selectivity of 100%. DBT is usually difficult to be oxidized for its steric hindrance effect.…”

Section: Catalysis For the Thioether Oxidization Reactionmentioning

confidence: 99%

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Recent progress of sub-1 nm nanomaterials: synthesis, polymer-analogue properties and applications in redox catalysis

Wang

Rong

2022

Chem. Commun.

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“…Thus, POM-based SNMs show high potential for TEO reaction catalysis. 70 selectivity of 100%. DBT is usually difficult to be oxidized for its steric hindrance effect.…”

Section: Catalysis For the Thioether Oxidization Reactionmentioning

confidence: 99%

“…We reported the fabrication of a 48 graphene-like POM-assembled structure, which was referred to as ''clusterphene''. 70 The hexagonal structure was constructed by the co-assembly of metal-substituted POM clusters (MPW 11 O 39 4À ) and quaternary ammonium cations (Fig. 8(a)).…”

Section: Catalysis For the Olefin Epoxidation Reactionmentioning

confidence: 99%

Recent progress of sub-1 nm nanomaterials: synthesis, polymer-analogue properties and applications in redox catalysis

Wang

Rong

2022

Chem. Commun.

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“…Two-dimensional (2D) materials have attracted extensive attention because of their unique structure-related potential in electronics, biomedicine, catalysis, and sensing and as membranes for separation and filtration. − Among various methods for rational design and synthesis of 2D organic materials, living seeded self-assembly has emerged as a powerful strategy for fabricating uniform 2D polymers with controlled shapes and sizes. Prominent examples are the block copolymer-based systems pioneered by Manners and coworkers, which have been successfully fabricated into uniform and complex 2D structures via crystallization-driven living self-assembly. − However, compared with polymers, living self-assembly of small molecules into uniform 2D structures with tailorable shapes and sizes remains a formidable challenge.…”

Section: Introductionmentioning

confidence: 99%

Unprecedented Small Molecule-Based Uniform Two-Dimensional Platelets with Tailorable Shapes and Sizes

Gong

Cheng

et al. 2022

J. Am. Chem. Soc.

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Fabrication of uniform two-dimensional (2D) structures from small molecules remains a formidable challenge for living self-assembly despite its great success in producing uniform one-dimensional (1D) structures. Here, we report the construction of unprecedented uniform 2D platelets with tailorable shapes and controlled sizes by creating new nuclei from a donor–acceptor (D–A) molecule and 1-hexanol to initiate 2D living self-assembly. We demonstrate that the D–A molecule undergoes 1-hexanol-induced twisting to form continuous alternative hydrogen bonds in-between under electrostatic attraction, which in turn forms a new nucleus. This connection architecture of the new nucleus allows to simultaneously regulate the growth rate of 1 in two dimensions to generate 2D platelets of distinct shapes through simply varying the amount of 1-hexanol relative to hexane. Furthermore, the living nature of the new nucleus enables seeded growth of complex concentric multiblock 2D heteroplatelets by sequential and alternative addition of different D–A molecules. Interestingly, the resulting 2D platelets obtained by such living self-assembly exhibit enhanced photostability compared to those obtained by conventional self-assembly without the involvement of 1-hexanol.

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“…Downsizing active species to a single-atom scale not only promotes the maximum atom utilization efficiency but also results in unique electronic properties for tuning binding strength with reaction intermediates. − Generally, the geometric and electronic structures of atomic metal sites can be engineered by their local coordination environment with other elements (O, B, S, P, etc. ). , However, it is difficult to modify the electronic structures merely through the introduction of heteroatoms due to the reason of the poor control of uniformity and dispersion. , Notably, controlling the long-range activation through interfacial interaction created by electron-donating/-withdrawing species can be a promising approach for tuning the electronic structure of single metal centers. − Sub-nanometric metal clusters exhibited excellent catalytic performance because of coordinatively unsaturated surface atoms, − resulting in electron delocalization and tunable electronic properties. , …”

Section: Introductionmentioning

confidence: 99%

Electronic Control of Traditional Iron–Carbon Electrodes to Regulate the Oxygen Reduction Route to Scale Up Water Purification

Wang

Xiao

Shen

et al. 2022

Environ. Sci. Technol.

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Shifting four-electron (4e–) oxygen reduction in fuel cell technology to a two-electron (2e–) pathway with traditional iron–carbon electrodes is a critical step for hydroxyl radical (HO•) generation. Here, we fabricated iron–carbon aerogels with desired dimensions (e.g., 40 cm × 40 cm) as working electrodes containing atomic Fe sites and Fe3C subnanoclusters. Electron-donating Fe3C provides electrons to FeN4 through long-range activation for achieving the ideal electronic configuration, thereby optimizing the binding energy of the *OOH intermediate. With an iron–carbon aerogel benefiting from finely tuned electronic density, the selectivity of 2e– oxygen reduction increased from 10 to 90%. The resultant electrode exhibited unexpectedly efficient HO• production and fast elimination of organics. Notably, the kinetic constant k M for sulfamethoxazole (SMX) removal is 60 times higher than that in a traditional iron–carbon electrode. A flow-through pilot device with the iron–carbon aerogel (SA-Fe0.4NCA) was built to scale up micropolluted water decontamination. The initial total organic carbon (TOC) value of micropolluted water was 4.02 mg L–1, and it declined and maintained at 2.14 mg L–1, meeting the standards for drinking water quality in China. Meanwhile, the generation of emerging aromatic nitrogenous disinfection byproducts (chlorophenylacetonitriles) declined by 99.2%, satisfying the public safety of domestic water. This work provides guidance for developing electrochemical technologies to satisfy the flexible and economic demand for water purification, especially in water-scarce areas.

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Self-assembly of polyoxometalate clusters into two-dimensional clusterphene structures featuring hexagonal pores

Cited by 93 publications

References 26 publications

Recent progress of sub-1 nm nanomaterials: synthesis, polymer-analogue properties and applications in redox catalysis

Recent progress of sub-1 nm nanomaterials: synthesis, polymer-analogue properties and applications in redox catalysis

Unprecedented Small Molecule-Based Uniform Two-Dimensional Platelets with Tailorable Shapes and Sizes

Electronic Control of Traditional Iron–Carbon Electrodes to Regulate the Oxygen Reduction Route to Scale Up Water Purification

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