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Sometimes the Same, Sometimes Different: Understanding Self-Assembly Algorithms in Coordination Networks.

Y Maximilian Klein1, Alessandro Prescimone2, Mariia Karpacheva3

  • 1Department of Chemistry, University of Basel, BPR 1096, Mattenstrasse 24a, 4058 Basel, Switzerland. maximilian.klein@psi.ch.

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Summary
This summary is machine-generated.

New ligands with two metal-binding domains were synthesized and characterized. Alkyloxy substituents on the ligands significantly influence the formation of 3D coordination networks, more so than the specific ligand isomer.

Keywords:
3,2′:6′,3″-terpyridine4,2′:6′,4″-terpyridinecobalt(II) thiocyanatemetal-organic frameworktetratopic ligands

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Area of Science:

  • Coordination Chemistry
  • Supramolecular Chemistry
  • Materials Science

Background:

  • Development of novel ligands with multiple metal-binding domains is crucial for constructing advanced coordination polymers and metal-organic frameworks.
  • The influence of functional groups on the self-assembly and structural diversity of coordination compounds is an active area of research.

Purpose of the Study:

  • To synthesize and characterize new bis-terpyridine ligands with varying alkyloxy functionalities.
  • To investigate the self-assembly behavior of these ligands with cobalt(II) thiocyanate.
  • To determine the impact of ligand structure and substituents on the resulting network topology.

Main Methods:

  • Ligand synthesis and characterization using standard organic chemistry techniques.
  • Crystallization of cobalt(II) complexes under ambient conditions.
  • Single crystal X-ray diffraction for structural determination.
  • Analysis of coordination modes and intermolecular interactions.

Main Results:

  • Three new ligands featuring two 4,2':6',4″-terpyridine or 3,2':6',3″-terpyridine metal-binding domains and diverse alkyloxy substituents were successfully synthesized.
  • Crystal structures of {[Co(NCS)₂(ligand 3)]·0.8C₆H₄Cl₂} and {[Co(NCS)₂(ligand 4)]·1.6H₂O·1.2C₆H₄Cl₂} revealed 3D cds net topologies, with both cobalt(II) centers and ligands acting as 4-connecting nodes.
  • The complex formed with ligand 5 and Co(NCS)₂ resulted in a discrete molecular complex [Co(NCS)₂(MeOH)₂(ligand 5)₂]·2CHCl₃·2MeOH, where ligand 5 acted as a monodentate ligand, showcasing efficient π-stacking interactions.

Conclusions:

  • The alkyloxy substituent on the phenylene spacer plays a more critical role in directing the formation of specific 3D network architectures than the isomeric form of the terpyridine unit.
  • Ligand design, particularly the nature of peripheral substituents, offers a powerful strategy for controlling the dimensionality and topology of coordination polymers.
  • The study highlights the intricate relationship between ligand structure, metal ion, and counterions in dictating the final supramolecular assembly.