Cu-Diketiminate
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Ammonia is a compelling candidate for a carbon-free energy carrier, offering potential applications asboth a hydrogen vector and a fuel. Unlocking these applications requires the development of efficientammonia oxidation catalysts. Building on recent work with a fluorinated Cu(I) β-diketiminate catalyst forhomogeneous ammonia oxidation, we present the first examples of hybrid electrodes employing first-row metal complexes and supramolecular anchoring for heterogeneous ammonia oxidation. In this study,we developed innovative synthetic methodologies to produce a family of β-diketiminate ligands and com-plexes. Some analogues clarified the role of each functional group in the original ligand, while othersincorporated moieties designed to facilitate immobilization on graphitic surfaces via CH–π and π–π inter-actions. These structural modifications not only broadened the scope of ligand design but also advancedour understanding of their roles in catalysis and immobilization. Unexpectedly, all synthesized Cu com-plexes, including the previously reported catalyst, formed an equilibrium with [CuI (NH3 )4 ]+ or[CuII(NH3)4 ] 2+ in the presence of ammonia, leading to ligand dissociation and subsequent catalyst de-activation. Despite these challenges, we demonstrated that anchoring these complexes is feasible andconfirmed that heterogeneous ammonia oxidation is possible with this system. This work represents apivotal step toward the construction of ammonia oxidation systems based on earth-abundant metals,highlighting the promise of Cu β-diketiminate complexes. Addressing the challenges of ligand loss andcatalyst stability will pave the way for robust and efficient systems, driving advancements in sustainableammonia-based energy technologies.
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Please use this identifier to cite or link to this collection:
DOI: 10.19061/iochem-bd-1-363
This dataset derived results are published in:
Manuscript title: Exploring copper β-diketiminate complexes for heterogeneous ammonia oxidation anchored on graphitic surfaces via CH–π and π–π interactions
Journal: Inorg. Chem. Front.
DOI: 10.1039/d5qi01170a
