Small molecule activation with bimetallic systems: a landscape of cooperative reactivity

Small molecule activation by well-defined compounds of heavy p-block elements.

Abstract The activation and functionalization of carbon dioxide entails great interest related to its abundance, low toxicity and associated environmental problems. However, the inertness of CO 2 has posed a challenge towards its efficient conversion to added‐value products. In this review we discuss one of the strategies that have been widely used to capture and activate carbon dioxide, namely the use of donor‐acceptor interactions by partnering a Lewis acidic and a Lewis basic fragment. This type of CO 2 activation resembles that found in metalloenzymes, whose outstanding performance in catalytically transforming carbon dioxide encourages further bioinspired research. We have divided this review into three general sections based on the nature of the active sites: metal‐free examples (mainly formed by frustrated Lewis pairs), main group‐transition metal combinations, and transition metal heterobimetallic complexes. Overall, we discuss one hundred compounds that cooperatively activate carbon dioxide by donor‐acceptor interactions, revealing a wide range of structural motifs. 

Donor-acceptor activation of Carbon Dioxide.

The rise of CO2 concentrations in the environment due to anthropogenic activities results in global warming and threatens the future of humanity and biodiversity. To address excessive CO2 emissions and...

Advances in CO2 Activation by Frustrated Lewis Pairs: From Stoichiometric to Catalytic Reactions

The Click reaction that involves Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) serves as the most potent and highly dependable tool for the development of many complex architectures. It has paved the way for the synthesis of numerous drug molecules with enhanced synthetic flexibility, reliability, specificity and modularity. It is all about bringing two different molecular entities together to achieve the required molecular properties. The utilization of Click chemistry has been well demonstrated in organic synthesis, particularly in reactions that involve biocompatible precursors. In pharmaceutical research, Click chemistry is extensively utilized for drug delivery applications. The exhibited bio-compatibility and dormancy towards other biological components under cellular environments makes Click chemistry an identified boon in bio-medical research. In this review, various click-derived transition metal complexes are discussed in terms of their applications and uniqueness. The scope of this chemistry towards other streams of applied sciences is also discussed.

Click-derived multifunctional metal complexes for diverse applications.

https://pubs.rsc.org/en/content/articlepdf/2022/cc/d2cc03089f

A highly constrained cis-dihydride platinum complex trapped by cooperative gold/platinum dihydrogen activation

The combination of molecular metallic fragments of contrasting Lewis character offers many possibilities for cooperative bond activation and for the disclosure of unusual reactivity. Here we provide a systematic investigation on the partnership of Lewis basic Rh(i) compounds of type [(η5-L)Rh(PR3)2] (η5-L = (C5Me5)− or (C9H7)−) with highly congested Lewis acidic Au(i) species. For the cyclopentadienyl Rh(i) compounds, we demonstrate the non-innocent role of the typically robust (C5Me5)− ligand through migration of a hydride to the Rh site and provide evidence for the direct implication of the gold fragment in this unusual bimetallic ligand activation event. This process competes with the formation of dinuclear Lewis adducts defined by a dative Rh → Au bond, with selectivity being under kinetic control and tunable by modifying the stereoelectronic and chelating properties of the phosphine ligands bound to the two metals. We provide a thorough computational study on the unusual Cp* non-innocent behavior and the divergent bimetallic pathways observed. The cooperative FLP-type reactivity of all bimetallic pairs has been investigated and computationally examined for the case of N–H bond activation in ammonia.

https://pubs.rsc.org/en/content/articlepdf/2023/dt/d3dt00410d

Polarized Au(i)/Rh(i) bimetallic pairs cooperatively trigger ligand non-innocence and bond activation

/pdf/a-genuine-germylene-pgep-pincer-ligand-for-formic-acid-8m01zksv.pdf

A genuine germylene PGeP pincer ligand for formic acid dehydrogenation with iridium.

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