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Metal-Ligand Bonds

Metal-Ligand Bonds

The hemoglobin in the blood, the chlorophyll in green plants, vitamin B-12, and the catalyst used in the manufacture of polyethylene all contain coordination compounds. Ions of the metals, especially the transition metals, are likely to form complexes.
In these complexes, transition metals form coordinate covalent bonds, a kind of Lewis acid-base interaction in which both of the electrons in the bond are contributed by a donor (Lewis base) to an electron acceptor (Lewis acid). The Lewis acid in...

Structural Isomerism

Structural Isomerism

Isomerism in Complexes
Isomers are different chemical species that have the same chemical formula. Structural isomerism of coordination compounds can be divided into two subcategories, the linkage isomers and coordination-sphere isomers.
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Valence Bond Theory

Valence Bond Theory

Coordination compounds and complexes exhibit different colors, geometries, and magnetic behavior, depending on the metal atom/ion and ligands from which they are composed. In an attempt to explain the bonding and structure of coordination complexes, Linus Pauling proposed the valence bond theory, or VBT, using the concepts of hybridization and the overlapping of the atomic orbitals. According to VBT, the central metal atom or ion (Lewis acid) hybridizes to provide empty orbitals of suitable...

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Color in Coordination Complexes
When atoms or molecules absorb light at the proper frequency, their electrons are excited to higher-energy orbitals. For many main group atoms and molecules, the absorbed photons are in the ultraviolet range of the electromagnetic spectrum, which cannot be detected by the human eye. For coordination compounds, the energy difference between the d orbitals often allows photons in the visible range to be absorbed and emitted, which is seen as colors by the human...

Complexation Equilibria: The Chelate Effect

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In complexation reactions, metal atoms or cations interact with ligands to form donor-acceptor adducts called metal complexes. Ligands that bind through one donor site are monodentate, ligands with two donor sites are bidentate, and those with more than two donor sites are polydentate ligands. For example, ethylene diamine is a bidentate ligand that binds through two nitrogen donor atoms, forming a five-membered ring. EDTA is a polydentate ligand that binds through four oxygen and two nitrogen...

Stereoisomerism

Stereoisomerism

Isomerism in Complexes
Isomers are different chemical species that have the same chemical formula.
Transition metal complexes often exist as geometric isomers, in which the same atoms are connected through the same types of bonds but with differences in their orientation in space. Coordination complexes with two different ligands in the cis and trans positions from a ligand of interest form isomers. For example, the octahedral [Co(NH3)4Cl2]+ ion has two isomers (Figure 1) In the cis...

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Updated: May 16, 2025

Preparation of SNS CobaltII Pincer Model Complexes of Liver Alcohol Dehydrogenase

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Cooperative Heterobimetallic CO₂ Activation Involving a Mononuclear Aluminum(II) Intermediate.

Roushan Prakash Singh¹, Kevin P Quirion², Joshua Telser³

¹Department of Chemistry, University of Illinois Chicago, Chicago, Illinois 60607, United States.

Journal of the American Chemical Society

|April 3, 2025

Summary

Transient aluminum(II) ions, previously underexplored, activate carbon dioxide (CO2) via a novel two-step reduction mechanism. This discovery opens new avenues for utilizing earth-abundant elements in unusual oxidation states for CO2 conversion.

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Published on: July 30, 2017

Area of Science:

Organometallic Chemistry
Inorganic Chemistry
Catalysis

Background:

Aluminum chemistry predominantly features the stable Al(III) oxidation state.
The reactivity and potential of the less common Al(II) oxidation state remain largely unexplored.
Understanding unusual oxidation states is key to discovering novel reaction pathways.

Purpose of the Study:

To investigate the carbon dioxide (CO2) activation chemistry of a transient Al(II) intermediate.
To elucidate the electronic structure and reaction mechanisms involved in Al(II)-mediated CO2 reduction.
To explore new reaction manifolds using earth-abundant elements in uncommon oxidation states.

Main Methods:

Synthesis and characterization of a heterobinuclear Al-Fe complex, (NON)Al-FeCp(CO)2.
In situ generation of a transient Al(II) species via Al-Fe bond homolysis.
Quantum-chemical calculations (DFT) and direct dynamics simulations to model reaction mechanisms.
Experimental validation using radical scavengers (TEMPO, benzophenone).

Main Results:

Ambient condition Al-Fe bond homolysis in (NON)Al-FeCp(CO)2 generates an Al(II) radical.
Predominantly Al-centered spin density confirmed for the Al(II) species.
CO2 insertion into the Al-Fe bond observed, leading to net 2-electron reduction.
Computational modeling revealed a two-step, one-electron reduction mechanism for CO2 activation.

Conclusions:

Transient Al(II) intermediates can effectively activate and reduce CO2 through a unique mechanism.
The reaction relies on the stabilization of the high-energy carbon dioxide radical anion ([CO2]•−) by aluminum coordination.
This work demonstrates the potential of earth-abundant elements in unusual oxidation states for novel chemical transformations.