Solvent‐Controlled Condensation of [Mo2O5(PTC4A)2]6− Metalloligand in Stepwise Assembly of Hexagonal and Rectangular Ag18 Nanoclusters

Wang, Zhi; Li, Li; Feng, Lei; Gao, Zhiyong; Tung, Chen‐Ho; Zheng, Lan‐Sun; Sun, Di

doi:10.1002/anie.202200823

Cited by 41 publications

(11 citation statements)

References 85 publications

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“…The results showed that the temperature of both compounds remarkably increased within 3 s at various power densities from 0.1 to 0.5 W cm –2 (Figure a). For example, at 0.5 W cm –2 , the temperature soared from 23 to 470 and 512 °C for Ag48M and Ag48T , respectively, and the corresponding heating rate (149 °C s –1 for Ag48M and 163 °C s –1 for Ag48T ) is much higher than most reported photothermal materials (Table S10), demonstrating the excellent photothermal conversion properties of both polymorphs . Before the measurement, the photothermal performance of Ag48M was expected to be better than that of Ag48T due to the weaker radiative decay (Figure S14).…”

Section: Resultsmentioning

confidence: 94%

Solvent-Mediated Separation and Reversible Transformation of 1D Supramolecular Polymorphs Built from [W₁₀O₃₂]^4– Templated 48-Nuclei Silver(I) Cluster

Sheng

Wang

et al. 2023

J. Am. Chem. Soc.

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Although the C−H•••O interaction is an essential component in determining the molecular packing in solids and the properties in supramolecular chemistry, it presents a significant challenge when trying to use it in the crystal engineering of complex metallosupramolecules, even though it is a relatively weak supramolecular force. The first pair of highnuclearity silver-cluster-based one-dimensional (1D) polymorphs built from supramolecular synthon [W 10 O 32 @Ag 48 (CyS) 24 (NO 3 ) 16 ]•4NO 3 (Cy = cyclohexyl) bridged by four grouped inorganic NO 3 − ligands is initially synthesized as a mixed phase and further individually crystallized as a pure phase by virtue of tuning intermolecular C−H•••O interaction through altering the composition ratio of ternary solvent system. Increasing highly polar and hydrogen-bonding methanol strengthens the solvation effect reflected by the change of coordination orientation of surface NO 3 − ligands, which dominates the packing of the 1D chains in the crystal lattice, resulting in the crystallization of polymorphs from tetragonal to monoclinic. The two crystalline forms can also be reversibly transformed to each other in an appropriate solvent system. Correspondingly, the two polymorphs display distinct temperature-dependent photoluminescence behaviors, which are ascribed to the variation of noncovalent interchain C−H••• O interactions along with the temperature. More importantly, benefiting from the suppression of fluorescence, both polymorphs offer excellent photothermal conversion properties which were further applied to remote-controlled laser ignition. These findings may open more avenues for the application of solvent-mediated intermolecular interaction in controlling the molecule arrangement as well as the optical properties.

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Section: Resultsmentioning

confidence: 94%

Solvent-Mediated Separation and Reversible Transformation of 1D Supramolecular Polymorphs Built from [W₁₀O₃₂]^4– Templated 48-Nuclei Silver(I) Cluster

Sheng

Wang

et al. 2023

J. Am. Chem. Soc.

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“…This is consistent with the distances in related silver clusters and almost identical to those in silver metal. [65] The whole structure of compound 1 shows an ellipsoidal shape. The central CO 3 2À ion plays a crucial role in building the structure of compound 1.…”

Section: Crystal Structure Description Of Compoundmentioning

confidence: 99%

Carboxylate Ligand‐supported Ag_n (n=21 and 24) Alkynyl Clusters Induced by Single/Double Carbonate Ions

Liu

Zhou

et al. 2023

Chemistry An Asian Journal

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Structural transformation is important for the study of silver cluster compounds, in which controlled synthesis of their shapes and sizes via anion template-driven is one key scientific question. In this work, the CO 3 2À anion templates were captured by the [ t BuC�CAg] n system under the stimulation induced by carboxylate ligand CF 3 COO À /PhCOO À , and two silver alkynyl clusters [(CO 3 2À )@Ag 21 ( t BuC�C) 16 (CF 3 COO) 3 (H 2 O)]•DMF•2CH 2 Cl 2 (1) and [(CO 3 2À ) 2 @Ag 24 ( t BuC�C) 16 (PhCOO) 4 ]•CH 3 OH•4DMF (2) have been successfully isolated and charactered. With the increase of the number of CO 3 2Àtemplates from single to double, the outer silver atoms from twenty-one to twenty-four, accompanied by the growth of the cluster skeleton from 9.8 Å × 6.9 Å of the (CO 3 2À )@Ag 21 unit to 10.5 Å × 7.3 Å of the (CO 3 2À ) 2 @Ag 24 unit. In addition, the syntheses, structures, photocurrent responses, cyclic voltammetry characteristics, luminescence, and photodegradation of compounds 1 and 2 have been studied.

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“…Thiacalix[4]arene (TC4A), which has many preorganized synergetic coordination sites compared to these ligands with a single coordination site, has a stiff shell that shields a metallic core and may have an added stabilizing impact on Ag NCs. However, most TC4A-protected Ag clusters were synthesized using oxoanions as templates, such as Ag 18 , Ag 36 , Ag 42 , Ag 47 , Ag 49 , and Ag 88 . − As far as we are aware, only four TC4A-protected Ag 1/0 superatoms, viz., Ag 21 , Ag 34 , and Ag 35 with eight valence electrons, ,, and Ag 155 with 92 valence electrons, have been structurally characterized until now . They are all in the closed-shell “magic” number series for valence electron numbers.…”

Section: Introductionmentioning

confidence: 99%

Unveiling the Remarkable Stability and Catalytic Activity of a 6-Electron Superatomic Ag₃₀ Nanocluster for CO₂ Electroreduction

Li,

Luo,

Tian

et al. 2023

Inorg. Chem.

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Nanocluster catalysts face a significant challenge in striking the right balance between stability and catalytic activity. Here, we present a thiacalix[4]arene-protected 6-electron [Ag30(TC4A)4(iPrS)8] nanocluster that demonstrates both high stability and catalytic activity. The Ag 30 nanocluster features a metallic core, Ag10 4+, consisting of two Ag3 triangles and one Ag4 square, shielded by four {Ag5@(TC4A)4} staple motifs. Based on DFT calculations, the Ag10 4+ metallic kernel can be viewed as a trimer comprising 2-electron superatomic units, exhibiting a valence electron structure similar to that of the Be3 molecule. Notably, this is the first crystallographic evidence of the trimerization of 2-electron superatomic units. Ag 30 can reduce CO2 into CO with a Faraday efficiency of 93.4% at −0.9 V versus RHE along with excellent long-term stability. Its catalytic activity is far superior to that of the chain-like AgI polymer ∞ 1{[H2Ag5(TC4A)(iPrS)3]} (∞ 1 Ag n ), with the composition similar to Ag 30 . DFT calculations elucidated the catalytic mechanism to clarify the contrasting catalytic performances of the Ag 30 and ∞ 1 Ag n polymers and disclosed that the intrinsically higher activity of Ag 30 may be due to the greater stability of the dual adsorption mode of the *COOH intermediate on the metallic core.

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Solvent‐Controlled Condensation of [Mo₂O₅(PTC4A)₂]⁶⁻ Metalloligand in Stepwise Assembly of Hexagonal and Rectangular Ag₁₈ Nanoclusters

Cited by 41 publications

References 85 publications

Solvent-Mediated Separation and Reversible Transformation of 1D Supramolecular Polymorphs Built from [W₁₀O₃₂]^4– Templated 48-Nuclei Silver(I) Cluster

Solvent-Mediated Separation and Reversible Transformation of 1D Supramolecular Polymorphs Built from [W₁₀O₃₂]^4– Templated 48-Nuclei Silver(I) Cluster

Carboxylate Ligand‐supported Ag_n (n=21 and 24) Alkynyl Clusters Induced by Single/Double Carbonate Ions

Unveiling the Remarkable Stability and Catalytic Activity of a 6-Electron Superatomic Ag₃₀ Nanocluster for CO₂ Electroreduction

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Solvent‐Controlled Condensation of [Mo2O5(PTC4A)2]6− Metalloligand in Stepwise Assembly of Hexagonal and Rectangular Ag18 Nanoclusters

Cited by 41 publications

References 85 publications

Solvent-Mediated Separation and Reversible Transformation of 1D Supramolecular Polymorphs Built from [W10O32]4– Templated 48-Nuclei Silver(I) Cluster

Solvent-Mediated Separation and Reversible Transformation of 1D Supramolecular Polymorphs Built from [W10O32]4– Templated 48-Nuclei Silver(I) Cluster

Carboxylate Ligand‐supported Agn (n=21 and 24) Alkynyl Clusters Induced by Single/Double Carbonate Ions

Unveiling the Remarkable Stability and Catalytic Activity of a 6-Electron Superatomic Ag30 Nanocluster for CO2 Electroreduction

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Solvent‐Controlled Condensation of [Mo₂O₅(PTC4A)₂]⁶⁻ Metalloligand in Stepwise Assembly of Hexagonal and Rectangular Ag₁₈ Nanoclusters

Solvent-Mediated Separation and Reversible Transformation of 1D Supramolecular Polymorphs Built from [W₁₀O₃₂]^4– Templated 48-Nuclei Silver(I) Cluster

Solvent-Mediated Separation and Reversible Transformation of 1D Supramolecular Polymorphs Built from [W₁₀O₃₂]^4– Templated 48-Nuclei Silver(I) Cluster

Carboxylate Ligand‐supported Ag_n (n=21 and 24) Alkynyl Clusters Induced by Single/Double Carbonate Ions

Unveiling the Remarkable Stability and Catalytic Activity of a 6-Electron Superatomic Ag₃₀ Nanocluster for CO₂ Electroreduction