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In most main group element compounds, the valence electrons of the isolated atoms combine to form chemical bonds that satisfy the octet rule. For instance, the four valence electrons of carbon overlap with electrons from four hydrogen atoms to form CH4. The one valence electron leaves sodium and adds to the seven valence electrons of chlorine to form the ionic formula unit NaCl (Figure 1a). Transition metals do not normally bond in this fashion. They primarily form coordinate covalent bonds, a...
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Accessing homoleptic neutral and anionic five-coordinate Pr(iv) siloxide complexes.

Pragati Pandey1, Megan Keener1, Thayalan Rajeshkumar2

  • 1Group of Coordination Chemistry, Institut des Sciences et Ingénierie Chimiques, École Polytechnique Fédérale de Lausanne (EPFL) CH-1015 Lausanne Switzerland marinella.mazzanti@epfl.ch.

Chemical Science
|October 15, 2025
PubMed
Summary
This summary is machine-generated.

New reaction conditions enable the synthesis of stable tetravalent praseodymium (Pr(iv)) complexes. This research details the isolation and characterization of novel Pr(iv) siloxide complexes, expanding the known examples of this challenging oxidation state.

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Area of Science:

  • Inorganic Chemistry
  • Organometallic Chemistry
  • Materials Science

Background:

  • Structurally characterized tetravalent praseodymium (Pr(iv)) complexes are rare due to the difficulty in stabilizing this oxidation state.
  • Existing research has identified only a limited number of Pr(iv) examples, highlighting the need for new synthetic strategies and stabilizing ligands.
  • The development of methods to access higher oxidation states in lanthanides is crucial for exploring their unique electronic and magnetic properties.

Purpose of the Study:

  • To identify specific reaction conditions and reagents that facilitate the synthesis and isolation of previously elusive Pr(iv) complexes.
  • To synthesize and fully characterize novel Pr(iv) complexes utilizing tris(tert-butoxy)siloxide and triphenylsiloxide ligands.
  • To investigate the influence of reaction parameters, such as oxidants and solvents, on the stability and isolation of high-valent Pr(iv) species.

Main Methods:

  • Oxidation of precursor praseodymium(iii) complexes using the thianthrene radical cation tetrafluoroborate (thiaBF4) oxidant.
  • Isolation and full characterization of the resulting Pr(iv) complexes, including [Pr(OSi(OtBu)3)4] (2-PrOtBu) and [MPr(OSiPh3)5] (5M-PrPh) (M = K, Cs).
  • Solid-state structural analysis, electrochemical studies, theoretical calculations, electron paramagnetic resonance (EPR), and SQUID magnetometry for characterization.

Main Results:

  • Successful synthesis and isolation of four new Pr(iv) complexes, including the first examples of anionic lanthanide(iv) complexes ([MPr(OSiPh3)5] and [KDB18C6][Pr(OSiPh3)5]).
  • Demonstration that specific reagents (thiaBF4 over magic blue) and non-coordinating solvents are critical for stabilizing Pr(iv).
  • Confirmation of the Pr(iv) oxidation state through a combination of spectroscopic, magnetic, structural, and electrochemical techniques.

Conclusions:

  • The study successfully establishes new reaction conditions for the synthesis of stable Pr(iv) complexes, significantly broadening the scope of known examples.
  • The development of anionic Pr(iv) complexes offers a new avenue for tuning redox potentials and accessing more stable high-valent lanthanide species.
  • This work provides a foundation for further exploration of high-valent lanthanide chemistry and their potential applications.