ArticleJournal of the American Chemical Society2013
Enhanced catalytic four-electron dioxygen (O2) and two-electron hydrogen peroxide (H2O2) reduction with a copper(II) complex possessing a pendant ligand pivalamido group.
Article in Journal of the American Chemical Society, 2013. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 19 papers.
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Who cites it
19 citing papers in PubMed, 112 citations in OpenAlex.
- Dimerization in TMPA-Based Copper(I) Complexes: Implications for Redox Kinetics and Thermodynamics.Inorganic chemistry · 2025Article
- Controlling outer-sphere solvent reorganization energy to turn on or off the function of artificial metalloenzymes.Nature communications · 2025Article
- Acid Strength Effects on Dimerization during Metal-Free Catalytic Dioxygen Reduction.Journal of the American Chemical Society · 2024Article
- Scaling Relation between the Reduction Potential of Copper Catalysts and the Turnover Frequency for the Oxygen and Hydrogen Peroxide Reduction Reactions.Inorganic chemistry · 2023Article
- Influence of the spatial distribution of copper sites on the selectivity of the oxygen reduction reaction.Dalton transactions (Cambridge, England : 2003) · 2022Article
- Electrocatalytic Oxygen Reduction to Produce Hydrogen Peroxide: Rational Design from Single-Atom Catalysts to Devices.Electrochemical energy reviews · 2022Review
- De Novo Design of a Self-Assembled Artificial Copper Peptide that Activates and Reduces Peroxide.ACS catalysis · 2021Article
- Mechanistic Study of the Activation and the Electrocatalytic Reduction of Hydrogen Peroxide by Cu-tmpa in Neutral Aqueous Solution.ChemElectroChem · 2021Article
- Influence of Ligand Denticity and Flexibility on the Molecular Copper Mediated Oxygen Reduction Reaction.Inorganic chemistry · 2020Article
- Copper(I) Complex Mediated Nitric Oxide Reductive Coupling: Ligand Hydrogen Bonding Derived Proton Transfer Promotes NJournal of the American Chemical Society · 2019Article
- Ligand Identity-Induced Generation of Enhanced Oxidative Hydrogen Atom Transfer Reactivity for a CuJournal of the American Chemical Society · 2019Article
- Synthetic Fe/Cu Complexes: Toward Understanding Heme-Copper Oxidase Structure and Function.Chemical reviews · 2018Review
- Light-induced formation of partially reduced oxygen species limits the lifetime of photosystem 1-based biocathodes.Nature communications · 2018Article
- Critical Aspects of Heme-Peroxo-Cu Complex Structure and Nature of Proton Source Dictate Metal-O(peroxo) Breakage versus Reductive O-O Cleavage Chemistry.Journal of the American Chemical Society · 2017Article
- One-Step Selective Hydroxylation of Benzene to Phenol with Hydrogen Peroxide Catalysed by Copper Complexes Incorporated into Mesoporous Silica-Alumina.Chemical science · 2016Article
- Laser-Induced Dynamics of Peroxodicopper(II) Complexes Vary with the Ligand Architecture. One-Photon Two-Electron O2 Ejection and Formation of Mixed-Valent Cu(I)Cu(II)-Superoxide Intermediates.Journal of the American Chemical Society · 2015Article
- Catalytic two-electron reduction of dioxygen catalysed by metal-free [14]triphyrin(2.1.1).Chemical science · 2015Article
- Lewis acid-induced change from four- to two-electron reduction of dioxygen catalyzed by copper complexes using scandium triflate.Journal of the American Chemical Society · 2015Article
- Nitric oxide generation from heme/copper assembly mediated nitrite reductase activity.Journal of biological inorganic chemistry : JBIC : a publication of the Society of Biological Inorganic Chemistry · 2014Article
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5 authors at 3 institutions in 3 countries.
Funding
Abstract
A copper complex, [(PV-tmpa)Cu(II)](ClO4)2 (1) [PV-tmpa = bis(pyrid-2-ylmethyl){[6-(pivalamido)pyrid-2-yl]methyl}amine], acts as a more efficient catalyst for the four-electron reduction of O2 by decamethylferrocene (Fc*) in the presence of trifluoroacetic acid (CF3COOH) in acetone as compared with the corresponding copper complex without a pivalamido group, [(tmpa)Cu(II)](ClO4)2 (2) (tmpa = tris(2-pyridylmethyl)amine). The rate constant (k(obs)) of formation of decamethylferrocenium ion (Fc*(+)) in the catalytic four-electron reduction of O2 by Fc* in the presence of a large excess CF3COOH and O2 obeyed first-order kinetics. The k(obs) value was proportional to the concentration of catalyst 1 or 2, whereas the k(obs) value remained constant irrespective of the concentration of CF3COOH or O2. This indicates that electron transfer from Fc* to 1 or 2 is the rate-determining step in the catalytic cycle of the four-electron reduction of O2 by Fc* in the presence of CF3COOH. The second-order catalytic rate constant (k(cat)) for 1 is 4 times larger than the corresponding value determined for 2. With the pivalamido group in 1 compared to 2, the Cu(II)/Cu(I) potentials are -0.23 and -0.05 V vs SCE, respectively. However, during catalytic turnover, the CF3COO(-) anion present readily binds to 2 shifting the resulting complex's redox potential to -0.35 V. The pivalamido group in 1 is found to inhibit anion binding. The overall effect is to make 1 easier to reduce (relative to 2) during catalysis, accounting for the relative k(cat) values observed. 1 is also an excellent catalyst for the two-electron two-proton reduction of H2O2 to water and is also more efficient than is 2. For both complexes, reaction rates are greater than for the overall four-electron O2-reduction to water, an important asset in the design of catalysts for the latter.
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