4.7 Article

Multi-State Dynamic Coordination Complexes Interconverted through Counterion-Controlled Phase Transfer

Journal

INORGANIC CHEMISTRY
Volume 60, Issue 7, Pages 4755-4763

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.0c03708

Keywords

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Funding

  1. National Science Foundation [CHE-1709888]
  2. Sherman Fairchild Foundation, Inc.
  3. Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF) [ECCS-1542205]
  4. State of Illinois
  5. International Institute for Nanotechnology (IIN)
  6. National Science Foundation Graduate Research Fellowship

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The study reveals that in a multiphasic solvent environment, dynamic weak-link approach (WLA) complexes demonstrated the ability to shuttle between aqueous and organic phases and modulate their denticity as they partition into different phases. This highly reconfigurable property of WLA complexes can be utilized to design biphasic reaction networks or chemical separations driven by straightforward salt metathesis reactions.
We studied a series of dynamic weak-link approach (WLA) complexes that can be shuttled between two immiscible solvents and switched between two structural states via ion exchange. Here, we established that hydrophobic anions transfer cationic, amphiphilic complexes from the aqueous phase to the organic phase, while a chloride source reverses the process. As a result of the dynamic metal coordination properties of WLA complexes, the denticity of these complexes (mono- to bi-) can be modulated as they partition into different phases. In addition, we discovered that heteroligated complexes bearing ligands of different donor strengths preferentially rearrange into two homoligated complexes that are phase-partitioned to maximize the number of stronger coordination bonds. This behavior is not observed in systems with one solvent, highlighting the dynamic and stimuli-responsive nature of hemilabile ligands in a multiphasic solvent environment. Taken together, this work shows that the highly reconfigurable WLA modality can enable the design of biphasic reaction networks or chemical separations driven by straightforward salt metathesis reactions.

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