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• W1998907685 abstract "The trinuclear nickel clusters [Ni3(μ2-dppm)3(μ3-L) (μ3-I)][PF6] (L = CNR, R = CH3 (1), i-C3H7 (2), C6H11 (3), CH2C6H5 (4), 1-C4H9 (5), 2,6-Me2C6H3 (6); L = CO (7); dppm = bis(diphenylphosphino)methane) undergo single electron reduction over a relatively narrow range of E1/2 (+/0) (− 1.08 to − 1.18 V versus SCE in acetonitrile) to form neutral radicals, [Ni3(μ2-dppm)3 (μ3-L) (μ3-I)]•. Specular reflectance IR spectroelectrochemical measurements were used to characterize these species and their reactions with CO2. Studies in the absence of CO2 show that the capping isocyanide or carbonyl ligand remains triply bridging (μ3,η1) upon single electron reduction. Electrochemical kinetics studies indicate that the rates of reaction with CO2 depend to first order on [cluster] and to first order on [CO2]. The rate constants for the rate limiting step in the reduction of CO2 by the clusters, kCO2 (M−1 s−1), are 1.6±0.3 (1), 1.4±0.3 (2), 0.5±0.1 (3), 0.2±0.05 (4), 0.0±0.05 (5), 0.0±0.05 (6), and 0.1±0.1 (7). Thus, the relative rates of reaction of the alkyl or aryl substituted isocyanide or carbonyl capped clusters with CO2 follow the order: CNCH3 (1) ∼ CN(i-C3H7) (2) > CNC6H11 (3) > CNCH2C6H5 (4) > CO (7) > CN (t-C4H9) (5) ∼ CN(2,6-Me2C6H3) (6). On the basis of these kinetic and spectroscopic studies, a mechanism for the catalytic reduction of CO2 involving CO2 activation on the isocyanide-capped face of the trinuclear nickel clusters is proposed." @default.
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• W1998907685 date "1998-04-01" @default.
• W1998907685 modified "2023-10-17" @default.
• W1998907685 title "Infrared spectroelectrochemical and electrochemical kinetics studies of the reaction of nickel cluster radicals [Ni3(μ2-dppm)3(μ3-L) (μ3I)]•(L = CNR, R = CH3, i-C3H7, C6H11, CH2C6H5, t-C4H9, 2,6-Me2C6H3; L = CO) with carbon dioxide" @default.
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• W1998907685 doi "https://doi.org/10.1016/s0020-1693(97)06097-0" @default.
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