Enhanced catalytic performance derived from coordination-driven structural switching between homometallic complexes and heterometallic polymeric materials

Kurpik, Gracjan; Walczak, Anna; Markiewicz, Grzegorz; Harrowfield, Jack; Stefankiewicz, Artur R.

doi:10.1039/d3nr01298k

Nanoscale

2023

DOI: 10.1039/d3nr01298k

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Enhanced catalytic performance derived from coordination-driven structural switching between homometallic complexes and heterometallic polymeric materials

Gracjan Kurpik

Anna Walczak

Grzegorz Markiewicz

et al.

Abstract: A bifunctional ligand 4,4-dimethyl-1-(pyridin-4-yl)pentane-1,3-dione (HL) able to provide two distinct coordination sites, i.e. anionic β-diketonate (after deprotonation) and neutral pyridine, has been used in the synthesis of Ag(I), Pd(II) and...

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Cited by 4 publications

References 46 publications

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Multi‐Stimuli‐Responsive Network of Multicatalytic Reactions using a Single Palladium/Platinum Catalyst

Kurpik,

Walczak,

Dydio

et al. 2024

Angewandte Chemie

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Given her unrivalled proficiency in the synthesis of all molecules of life, nature has been an endless source of inspiration for developing new strategies in organic chemistry and catalysis. However, one feature that remains beyond chemists’ grasp is her unique ability to adapt the productivity of metabolic processes in response to triggers that indicate the temporary need for specific metabolites. To demonstrate the remarkable potential of such stimuli‐responsive systems, we present a metabolism‐inspired network of multicatalytic processes capable of selectively synthesising a range of products from simple starting materials. Specifically, the network is built of four classes of distinct catalytic reactions – cross‐couplings, substitutions, additions, and reductions, involving three organic starting materials – terminal alkyne, aryl iodide, and hydrosilane. All starting materials are either introduced sequentially or added to the system at the same time, with no continuous influx of reagents or efflux of products. All processes in the system are catalysed by a multifunctional heteronuclear PdII/PtII complex, whose performance can be controlled by specific additives and external stimuli. The reaction network exhibits a substantial degree of orthogonality between different pathways, enabling the controllable synthesis of ten distinct products with high efficiency and selectivity through simultaneous triggering and suppression mechanisms.

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Multi‐Stimuli‐Responsive Network of Multicatalytic Reactions using a Single Palladium/Platinum Catalyst

Kurpik,

Walczak,

Dydio

et al. 2024

Angewandte Chemie

View full text Add to dashboard Cite

show abstract

Multi‐Stimuli‐Responsive Network of Multicatalytic Reactions using a Single Palladium/Platinum Catalyst

Kurpik,

Walczak,

Dydio

et al. 2024

Angew Chem Int Ed

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Crafting Versatile Modes of Pt(II) Complexes with Flexidentate Pyridyl‐β‐diketones: Synthesis, Structural Characterization, and Catalytic Behavior in Olefin Hydrosilylation

Kurpik,

Walczak,

Łukasik

et al. 2023

ChemCatChem

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Cycloplatinated complexes, with their high reactivity, combined with the capability to tailor ligands for specific catalytic processes, play a pivotal role in materials science and coordination chemistry, serving as versatile catalysts for applications in the organic synthesis of industrially relevant processes. In this report, we describe the synthesis and characterization of a new family of Pt(II) complexes based on three isomeric pyridyl‐β‐diketones diversified in terms of N‐atom location in the heterocyclic ring. By appropriate control of the reaction conditions, we were able to generate distinct coordination species, featuring ligands arranged as N,C(sp3)‐ and N,O‐chelates, as well as simple pyridyl‐N donors. Various analytical techniques, including X‐Ray diffraction, NMR spectroscopy and ESI‐MS spectrometry enabled the characterization of different coordination modes of the central atoms and unambiguously established the complex structures. Furthermore, all the Pt(II) coordination units have been found to be highly active and selective catalyst precursors in the hydrosilylation reactions within a broad scope of olefins with hydrosilanes.

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Enhanced catalytic performance derived from coordination-driven structural switching between homometallic complexes and heterometallic polymeric materials

Abstract: A bifunctional ligand 4,4-dimethyl-1-(pyridin-4-yl)pentane-1,3-dione (HL) able to provide two distinct coordination sites, i.e. anionic β-diketonate (after deprotonation) and neutral pyridine, has been used in the synthesis of Ag(I), Pd(II) and...

Cited by 4 publications

References 46 publications

Multi‐Stimuli‐Responsive Network of Multicatalytic Reactions using a Single Palladium/Platinum Catalyst

Multi‐Stimuli‐Responsive Network of Multicatalytic Reactions using a Single Palladium/Platinum Catalyst

Multi‐Stimuli‐Responsive Network of Multicatalytic Reactions using a Single Palladium/Platinum Catalyst

Crafting Versatile Modes of Pt(II) Complexes with Flexidentate Pyridyl‐β‐diketones: Synthesis, Structural Characterization, and Catalytic Behavior in Olefin Hydrosilylation

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