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Catalytic Scavenging of Plant Reactive Oxygen Species In Vivo by Anionic Cerium Oxide Nanoparticles

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Two-Electron Oxidations at a Single Cerium Center.

Yi Wang¹, Jiefeng Liang¹, Chong Deng¹

¹Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China.

Journal of the American Chemical Society

|September 22, 2023

Summary

Researchers achieved two-electron oxidations at a single cerium(II) center, creating novel cerium(IV) oxo and imido complexes. This breakthrough expands the possibilities in rare-earth metal chemistry and catalysis.

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Area of Science:

Inorganic Chemistry
Organometallic Chemistry
Rare-Earth Metal Science

Background:

Two-electron oxidations are crucial in synthesis and catalysis, typically occurring at single transition metal or actinide sites.
Rare-earth metal redox chemistry has been restricted to one-electron processes due to limited accessible oxidation states and instability of low-valent compounds.

Purpose of the Study:

To achieve and characterize two-electron oxidation processes at a single rare-earth metal center.
To explore the synthesis and electronic structure of novel cerium complexes across different oxidation states.

Main Methods:

Synthesis and characterization of a series of cerium(II-IV) complexes using a tripodal tris(amido)arene ligand.
Experimental and theoretical studies (e.g., spectroscopy, X-ray crystallography, DFT calculations) to elucidate electronic structures and bonding.

Main Results:

Successful synthesis of cerium(II) complexes stabilized by δ-backdonation, described as 4f² ions.
Demonstration of two-electron oxidation from cerium(II) to cerium(IV) to form terminal oxo and imido complexes.
Characterization of cerium(IV) oxo and imido complexes, revealing multiple bonding interactions.

Conclusions:

This work demonstrates the feasibility of two-electron oxidation at a single rare-earth metal center, specifically cerium.
The findings introduce a new dimension to molecular rare-earth metal chemistry, challenging previous limitations.
The developed cerium complexes offer new avenues for catalytic applications and fundamental studies in redox chemistry.