Visualizing the Hierarchical Evolution of Aryl–Metal Bonding in Organometallic Nanostructures on Ag(111)

Gao, Yuhong; Zhang, Zhaoyu; Yi, Zewei; Zhang, Chi; Xu, Wei

doi:10.1021/acs.jpclett.3c02950

Cited by 3 publications

(1 citation statement)

References 29 publications

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“…Based on the submolecularly resolved STM image, an organometallic dimer structure with a Au adatom linking two molecular components via C–Au contacts was calculated. The DFT-optimized structural model (left and bottom panels of Figure c) shows that two DBIBP molecules are connected via a Au adatom located in the bay region by forming four C–Au contacts as a result of deiodination, , while four Br substituents remain in the termini, in good agreement with the hierarchical dehalogenation scenario as reported. − Accordingly, the STM simulation (right) successfully reproduces the experimental topography. The small bright dots around the H-motifs are thus assigned to the dissociated iodine atoms.…”

Section: Resultsmentioning

confidence: 99%

Separation of Halogen Atoms by Sodium from Dehalogenative Reactions on a Au(111) Surface

Zhang,

Gao,

et al. 2024

ACS Nano

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On-surface dehalogenative reactions have been promising in the construction of nanostructures with diverse morphologies and intriguing electronic properties, while halogen (X), as the main byproduct, often impedes the formation of extended nanostructures and property characterization, and the reaction usually requires high C−X activation temperatures, especially on relatively inert Au(111). Enormous efforts in precursor design, halogen-to-halide conversion, and the introduction of extrinsic metal atoms have been devoted to either eliminating dissociated halogens or reducing reaction barriers. However, it is still challenging to separate halogens from molecular systems while facilitating C−X activation under mild conditions. Herein, a versatile halogen separation strategy has been developed based on the introduction of extrinsic sodium (Na) into dehalogenative reactions on Au(111) as model systems that both isolates the dissociated halogens and facilitates the C−Br activation under mild conditions. Moreover, the combination of scanning tunneling microscopy imaging and density functional theory calculations reveals the formation of sodium halides (NaX) from halogens in these separation processes as well as the reduction in reaction temperatures and barriers, demonstrating the versatility of extrinsic sodium as an effective "cleaner" and "dehalogenator" of surface halogens. Our study demonstrates a valuable strategy to facilitate the on-surface dehalogenative reactions, which will assist in the precise fabrication of low-dimensional carbon nanostructures.

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Section: Resultsmentioning

confidence: 99%

Separation of Halogen Atoms by Sodium from Dehalogenative Reactions on a Au(111) Surface

Zhang,

Gao,

et al. 2024

ACS Nano

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Multiple Interaction Forces Construct Two‐Dimensional Self‐assembly Kagome Lattices on Au(111)

Zhang,

Lu,

Gao

et al. 2024

Chin. J. Chem.

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Comprehensive SummaryKagome lattices have garnered significant attention due to their promising applications in catalysis, electronics, and magnetics. Although many efforts have been paid to the design and synthesis of Kagome lattices, there is a limited focus on constructing this lattice by multiple interaction forces. In this work, we employ 2,7‐dibromo‐carbazole as precursors to successfully fabricate the two‐dimensional self‐assembly Kagome lattices stabled by multiple interaction forces on Au(111) substrate. Using low‐temperature scanning tunneling microscopy, non‐contact atomic force microscopy and density functional theory calculation, we visualize and identify the four interaction forces within Kagome lattices: Au—N coordination bonds, Au—H hydrogen bonds, Br—Br halogen bonds, and Br—H hydrogen bonds, respectively. This study provides a basic understanding for designing and constructing more complex Kagome lattices.

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Controlling the Selectivity of Reaction Products by Transmetalation on a Ag(111) Substrate

Xu,

Zhang,

Hou

et al. 2024

J. Phys. Chem. Lett.

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On-surface synthesis has shown great promise in the precise bottom-up preparation of molecular nanostructures. Apart from the direct C−C coupling reaction pathway, an alternative strategy is to exploit the metal−organic interactions provided by integrated metals for preassembly, which exhibit high reversibility and can anchor specific conformations of molecular precursors, thus allowing the precise construction of nanostructures with improved reaction selectivity. Previous studies have mainly been devoted to the construction of target reaction products through the incorporation of metal atoms, ranging from intrinsic to extrinsic atoms on metal substrates and, more recently, to their cooperative effects. However, the formation of different covalent nanostructures by competitive interactions between intrinsic and extrinsic adatoms remains elusive. Herein, we controlled the selectivity of covalent reaction products from isomerically specific transchains to cis-rings, resulting from the transmetalation of intrinsic Ag adatoms to extrinsic Na atoms on a Ag(111) substrate. Our results exhibit the competitive interactions between intrinsic and extrinsic metal atoms in real space and demonstrate their influence on the selectivity of reaction products, which should broaden the regulatory strategies for on-surface synthesis that shed light on the controllable and selective synthesis of target covalent nanostructures.

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Visualizing the Hierarchical Evolution of Aryl–Metal Bonding in Organometallic Nanostructures on Ag(111)

Cited by 3 publications

References 29 publications

Separation of Halogen Atoms by Sodium from Dehalogenative Reactions on a Au(111) Surface

Separation of Halogen Atoms by Sodium from Dehalogenative Reactions on a Au(111) Surface

Multiple Interaction Forces Construct Two‐Dimensional Self‐assembly Kagome Lattices on Au(111)

Controlling the Selectivity of Reaction Products by Transmetalation on a Ag(111) Substrate

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