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The molecular tetravalent oxidation state for praseodymium is observed in solution via oxidation of the anionic trivalent precursor [K][Pr 3+ (NP(1,2-bis- t Bu-diamidoethane)(NEt 2 )) 4 ] (1-Pr(NP*)) with AgI at −35 °C. The Pr 4+ complex is characterized in solution via cyclic voltammetry, UV-vis-NIR electronic absorption spectroscopy, and EPR spectroscopy. Electrochemical analyses of [K][Ln 3+ (NP(1,2-bis- t Bu-diamidoethane)(NEt 2 )) 4 ] (Ln = Nd and Dy) by cyclic voltammetry are reported and, in conjunction with theoretical modeling of electronic structure and oxidation potential, are indicative of principal ligand oxidations in contrast to the metal-centered oxidation observed for 1-Pr(NP*).more »Free, publicly-accessible full text available May 3, 2023
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Reaction of the complexes [Fe 2 (μ 2 -NP(pip) 3 ) 2 (NP(pip) 3 ) 2 ] ( 1-Fe ) and [Co 2 (μ 2 -NP(pip) 3 ) 2 (NP(pip) 3 ) 2 ] ( 1-Co ), where [NP(pip) 3 ] 1− is tris(piperidinyl)imidophosphorane, with nitrous oxide, S 8 , or Se 0 results in divergent reactivity. With nitrous oxide, 1-Fe forms [Fe 2 (μ 2 -O)(μ 2 -NP(pip) 3 ) 2 (NP(pip) 3 ) 2 ] ( 2-Fe ), with a very short Fe 3+ –Fe 3+ distance. Reactions of 1-Fe with S 8 or Se 0 result inmore »
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Free, publicly-accessible full text available July 1, 2023
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Here we report measurements of the oxygen reduction reaction (ORR) at single Pt nanoparticles (NPs) through their collision with a Au microdisk electrode of lower electrocatalytic activity. Performing measurements at an elevated pressure (10-atm, pure O2) raises the O2concentration ∼50-fold over air-saturated measurements, allowing the ORR activity of smaller Pt NPs to be resolved and quantified, compared to measurements taken at atmospheric pressure. Single-NP ORR current vs potential measurements for 2.6, 16, and 24 nm radius citrate-capped Pt NPs, show the catalytic activity of the smallest Pt NPs to be roughly one order of magnitude greater than the activity ofmore »