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Ion Exchange01:17

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Ion exchange chromatography separates charged molecules from a solution by reversibly exchanging them with mobile, or 'active', ions associated with the oppositely charged stationary phase. This method can be used to separate ions, soften and deionize water, and purify solutions. The polymers comprising the ion-exchange column are high-molecular-weight and chemically stable polymers, crosslinked to be porous and essentially insoluble. They are also functionalized with either acidic or...
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In 1923, G. N. Lewis proposed a generalized definition of acid-base behavior in which acids and bases are identified by their ability to accept or to donate a pair of electrons and form a coordinate covalent bond.
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This lesson delves into Lewis acids and bases in the context of the octet rule for electron-deficient compounds. Here, the concept is discussed, emphasizing the group 13 elements like boron or aluminium. Since group 13 elements possess three valence electrons, they form trivalent compounds with a sextet of electrons and a vacant orbital for the central atom. Consequently, these electron-deficient compounds accept electrons from other species to complete their octet in a chemical reaction. They...
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An understanding of the solvating effect helps rationalize the relation between solvation and acidity of the compound. In addition, this also explains the relative stability of conjugate bases for compounds with different pKa values. This lesson details, in-depth, the principle of solvating effects. The strength of an acid and the stability of its corresponding conjugate base are determined using pKa values. This observed relationship is a consequence of solvation, which is the interaction...
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Fabrication and Optimization of Type II Silicon Clathrate Films
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Isolable Silicon-Based Polycations with Lewis Superacidity.

André Hermannsdorfer1, Matthias Driess1

  • 1Department of Chemistry: Metalorganics and Inorganic Materials, Technische Universität Berlin, Strasse des 17. Juni 115, Sekr. C2, 10623, Berlin, Germany.

Angewandte Chemie (International Ed. in English)
|September 16, 2020
PubMed
Summary

Researchers synthesized stable silicon polycations, [R2Si(terpy)]2+ and [RSi(terpy)]3+, which act as potent Lewis superacids. These novel compounds demonstrate reactivity towards C(sp3)-F bonds, enabling fluoride abstraction and catalytic hydrodefluorination reactions.

Keywords:
Coordination compoundsHydride transferHydrodefluorinationMain group elementsSilanes

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Light Enhanced Hydrofluoric Acid Passivation: A Sensitive Technique for Detecting Bulk Silicon Defects
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Area of Science:

  • Organosilicon Chemistry
  • Superacid Catalysis
  • Coordination Chemistry

Background:

  • Molecular silicon polycations (R2Si2+ and RSi3+) are theoretically predicted Lewis superacids but remain largely unknown in condensed phases.
  • Stabilization of highly charged silicon centers presents a significant synthetic challenge.

Purpose of the Study:

  • To synthesize and characterize isolable terpyridine-stabilized silicon polycations of the types [R2Si(terpy)]2+ and [RSi(terpy)]3+.
  • To investigate the Lewis superacidic properties and reactivity of these novel silicon complexes.
  • To demonstrate their ability to activate and cleave strong chemical bonds, such as C(sp3)-F bonds.

Main Methods:

  • Synthesis of terpyridine-stabilized silicon polycation complexes ([R2Si(terpy)]2+ and [RSi(terpy)]3+) as triflate salts.
  • Characterization using spectroscopic and crystallographic techniques.
  • Experimental and theoretical evaluation of Lewis superacidity and fluoride/hydride ion affinities.
  • Demonstration of stoichiometric fluoride abstraction from 1-fluoroadamantane and catalytic hydrodefluorination.

Main Results:

  • Successful synthesis and isolation of a series of terpyridine-stabilized R2Si2+ and RSi3+ complexes.
  • Confirmation of retained Lewis superacidic character in the synthesized silicon polycations, despite reduced fluoride ion affinities in higher-coordinate species.
  • Demonstration of C(sp3)-F bond activation via stoichiometric fluoride abstraction from 1-fluoroadamantane.
  • Catalytic hydrodefluorination of 1-fluoroadamantane using the synthesized silicon complexes.
  • Isolation of crystalline adducts with fluoride and hydride donors, confirming high reactivity.

Conclusions:

  • Terpyridine ligation enables the isolation of previously elusive molecular silicon polycations in the condensed phase.
  • These silicon polycations exhibit significant Lewis superacidic behavior, capable of activating robust C(sp3)-F bonds.
  • The developed complexes represent a new class of reagents for defluorination reactions and hold potential for broader applications in catalysis.