Enhanced catalytic performance derived from coordination-driven structural switching between homometallic complexes...

Area of Science:

• Coordination Chemistry
• Supramolecular Chemistry
• Materials Science
• Catalysis

Background:

• Development of versatile ligands for constructing complex metal-based architectures.
• Exploration of bifunctional ligands with distinct coordination sites for tunable properties.
• Need for efficient catalytic systems derived from metallosupramolecular materials.

Purpose of the Study:

• To synthesize and characterize novel Ag(I), Pd(II), and Pt(II) complexes using a bifunctional ligand.
• To investigate the ligand's ability to form mononuclear complexes and heterometallic polymeric materials.
• To evaluate the catalytic activity of the synthesized palladium-based assemblies in the Heck cross-coupling reaction.

Main Methods:

• Synthesis of a bifunctional ligand: 4,4-dimethyl-1-(pyridin-4-yl)pentane-1,3-dione (HL).
• Formation of metal complexes and subsequent self-assembly into polymeric materials.
• Characterization using solution techniques (1H NMR, ESI-MS) and solid-state methods (XPS, SEM-EDS, FTIR, pXRD, TGA).

Main Results:

• Successful synthesis of Ag(I), Pd(II), and Pt(II) complexes and heterometallic polymeric materials.
• Demonstration of controllable coordination modes and stimuli-responsive self-assembly.
• Pd-based assemblies exhibited efficient catalytic activity in the Heck cross-coupling reaction.

Conclusions:

• The bifunctional ligand enables the controllable synthesis of diverse metallosupramolecular materials.
• The coordination-driven self-assembly strategy is effective for generating multimetallic coordination aggregates.
• The catalytic performance is influenced by the composition and morphology of the Pd-based assemblies.