Ultrastable and Highly Catalytically Active N‐Heterocyclic‐Carbene‐Stabilized Gold Nanoparticles in Confined Spaces

Gou, Xing‐Xing; Liu, Tong; Wang, Yao‐Yu; Han, Ying‐Feng

doi:10.1002/ange.202006569

Cited by 18 publications

(1 citation statement)

References 105 publications

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“…The B−H•••π interactions have also been observed in the B−H•••benzene system. 28 These interactions intrinsically diminish the π-accepting properties of the carbene ligands.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Nickelacarborane-Supported Bis-N-heterocyclic Carbenes

Nan

Zhu

et al. 2023

J. Am. Chem. Soc.

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Metallacarboranes have attracted significant attention due to their unique properties. Considerable efforts have been made on the reactions around the metal centers or the metal ion itself, while transformations of functional groups of the metallacarboranes have been much less explored. We presented here the formation of imidazoliumfunctionalized nickelacarboranes (2), their subsequent conversion to nickelacarborane-supported N-heterocyclic carbenoids (NHCs, 3), and the reactivities of 3 toward Au(PPh 3 )Cl and Se powder, which resulted in the formation of bis-gold carbene complexes (4) and NHC selenium adducts (5). Cyclic voltammetry of 4 shows two reversible peaks, corresponding to the interconversion transformations Ni II ↔ Ni III and Ni III ↔ Ni IV . Theoretical calculations demonstrated relatively high-lying lone-pair orbitals, weak B−H•••H−C interactions between the BH units and the methyl group, and weak B−H•••π interactions between the BH groups and the vacant p-orbital of the carbene.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Nickelacarborane-Supported Bis-N-heterocyclic Carbenes

Nan

Zhu

et al. 2023

J. Am. Chem. Soc.

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Mit N‐heterocyclischen Carbenen funktionalisierte Poly(3‐hexylthiophene) als robuste und leitfähige Liganden zur Stabilisierung von Goldnanopartikeln

et al. 2020

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Seit kurzem werden N‐heterocyclische Carbene (NHCs) als Ankergruppen verwendet, um organische Liganden an kolloidales Gold (d. h. Goldnanopartikel, Au NPs) zu binden. Die Arbeiten beschränken sich jedoch bisher auf nicht‐konjugierte Liganden, konzentrieren sich also allein auf die Ausnutzung des Stabilitätsaspekts. Bei der Verwendung von NHCs zur Verknüpfung von Au NPs mit elektronisch aktiven organischen Komponenten (z. B. konjugierten Polymeren, KPs) könnten sowohl die Stabilität als auch die inhärente Leitfähigkeit der NHC‐Anker genutzt werden. Hier berichten wir über drei Arten von Br‐NHC‐Au‐X‐Komplexen (X=Cl, Br). Ausgehend von diesen kann über Kumada‐Polykondensation regioreguläres Poly(3‐hexylthiophen)‐NHC‐Au (P3HTs‐NHC‐Au) mit engen Molmassenverteilungen erhalten werden. Die entsprechenden NPs werden durch direkte Reduktion erhalten und zeigen eine ausgezeichnete thermische und Redoxstabilität. Die NHC‐Anker ermöglichen die Delokalisierung von Elektronen über die Gold/KP‐Grenzfläche, was zu einem verbesserten elektrochromen Reaktionsverhalten gegenüber dem von P3HT‐NHC‐Au führt.

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N‐Heterocyclic Carbene‐Stabilized Ultrasmall Gold Nanoclusters in a Metal‐Organic Framework for Photocatalytic CO₂Reduction

Jiang

Zhang

et al. 2021

Angewandte Chemie

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Ultrafine gold nanoclusters (Au‐NCs) are susceptible to migrate and aggregate, even in the porosity of many crystalline solids. N‐heterocyclic carbenes (NHCs) are a class of structurally diverse ligands for the stabilization of Au‐NCs in homogeneous chemistry, showing catalytic reactivity in CO2 activation. Herein, for the first time, we demonstrate a heterogeneous nucleation approach to stabilize ultrasmall and highly dispersed gold nanoclusters in an NHC‐functionalized porous matrix. The sizes of gold nanoclusters are tunable from 1.3 nm to 1.8 nm based on the interpenetration of the metal‐organic framework (MOF) topology. Control experiments using amine or imidazolium‐functionalized MOFs afforded the aggregation of Au species. The resultant Au‐NC@MOF composite exhibits a steady and excellent activity in photocatalytic CO2 reduction, superior to control mixtures without NHC‐ligand stabilization. Mechanistic studies reveal the synergistic catalytic effect of MOFs and Au‐NCs through the MOF‐NHC‐Au covalent‐bonding bridges.

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Ultrastable and Highly Catalytically Active N‐Heterocyclic‐Carbene‐Stabilized Gold Nanoparticles in Confined Spaces

Cited by 18 publications

References 105 publications

Nickelacarborane-Supported Bis-N-heterocyclic Carbenes

Nickelacarborane-Supported Bis-N-heterocyclic Carbenes

Mit N‐heterocyclischen Carbenen funktionalisierte Poly(3‐hexylthiophene) als robuste und leitfähige Liganden zur Stabilisierung von Goldnanopartikeln

N‐Heterocyclic Carbene‐Stabilized Ultrasmall Gold Nanoclusters in a Metal‐Organic Framework for Photocatalytic CO₂Reduction

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Ultrastable and Highly Catalytically Active N‐Heterocyclic‐Carbene‐Stabilized Gold Nanoparticles in Confined Spaces

Cited by 18 publications

References 105 publications

Nickelacarborane-Supported Bis-N-heterocyclic Carbenes

Nickelacarborane-Supported Bis-N-heterocyclic Carbenes

Mit N‐heterocyclischen Carbenen funktionalisierte Poly(3‐hexylthiophene) als robuste und leitfähige Liganden zur Stabilisierung von Goldnanopartikeln

N‐Heterocyclic Carbene‐Stabilized Ultrasmall Gold Nanoclusters in a Metal‐Organic Framework for Photocatalytic CO2Reduction

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N‐Heterocyclic Carbene‐Stabilized Ultrasmall Gold Nanoclusters in a Metal‐Organic Framework for Photocatalytic CO₂Reduction