Abstract:Cyclic voltammetry and bulk electrolysis showed that [Ni(II)(salphen)] [1], [Ni(II)(tBu-salphen)] [2], and a binuclear Ni(II) compound combining salphen and tBu-salphen [3] react with CO2 to yield a metal-carbonyl species that...
“…[22,23] As a rule, molecular nickel-based electrocatalysts typically convert CO 2 into CO/H 2 O, CO 3 2À , or C 2 O 4 2À with either high or moderate faradaic efficiency. [24][25][26][27][28][29][30] As is known, the reaction of reducing CO 2 to CH 4 requires four electrons and four protons. Moreover, the potential of this reaction is high and lies within the area of the competition reaction, i. e., hydrogen evolution.…”
Section: Introductionmentioning
confidence: 99%
“…However, homogeneous Ni–based electrocatalysts with the capability to convert CO 2 into CH 4 are exceptionally rare [22,23] . As a rule, molecular nickel–based electrocatalysts typically convert CO 2 into CO/H 2 O, CO 3 2− , or C 2 O 4 2− with either high or moderate faradaic efficiency [24–30] …”
Processing CO2 into value‐added chemicals and fuels stands as one of the most crucial tasks in addressing the global challenge of the greenhouse effect. In this study, we focused on the complex (dpp‐bian)NiBr2 (where dpp‐bian is di‐isopropylphenyl bis‐iminoacenaphthene) as a precatalyst for the electrochemical reduction of CO2 into CH4 as the sole product. Cyclic voltammetry results indicate that the realization of a catalytically effective pattern requires the three‐electron reduction of (dpp‐bian)NiBr2. The chemically reduced complexes [K(THF)6]+[(dpp‐bian)Ni(COD)]– and [K(THF)6]+[(dpp‐bian)2Ni]– were synthesized and structurally characterized. Analyzing the data from the electron paramagnetic resonance study of the complexes in a solution, along with quantum‐chemical calculations, reveals that the spin density is predominantly localized at their metal centers. The superposition of trajectory maps of the electron density gradient field and the one‐electron electrostatic force field, along with the atomic charges, discloses that, within the first coordination sphere, the interatomic charge transfer occurs from the metal atom to the ligand atoms and that the complex anions can thus be formally described by the general formulas (dpp‐bian)2–Ni+(COD) and (dpp‐bian)2–Ni+. It was shown that the reduced nickel complexes can be oxidized by formic acid; resulting from this reaction, the two‐electron and two‐proton addition product dpp‐bian‐2H is formed.
“…[22,23] As a rule, molecular nickel-based electrocatalysts typically convert CO 2 into CO/H 2 O, CO 3 2À , or C 2 O 4 2À with either high or moderate faradaic efficiency. [24][25][26][27][28][29][30] As is known, the reaction of reducing CO 2 to CH 4 requires four electrons and four protons. Moreover, the potential of this reaction is high and lies within the area of the competition reaction, i. e., hydrogen evolution.…”
Section: Introductionmentioning
confidence: 99%
“…However, homogeneous Ni–based electrocatalysts with the capability to convert CO 2 into CH 4 are exceptionally rare [22,23] . As a rule, molecular nickel–based electrocatalysts typically convert CO 2 into CO/H 2 O, CO 3 2− , or C 2 O 4 2− with either high or moderate faradaic efficiency [24–30] …”
Processing CO2 into value‐added chemicals and fuels stands as one of the most crucial tasks in addressing the global challenge of the greenhouse effect. In this study, we focused on the complex (dpp‐bian)NiBr2 (where dpp‐bian is di‐isopropylphenyl bis‐iminoacenaphthene) as a precatalyst for the electrochemical reduction of CO2 into CH4 as the sole product. Cyclic voltammetry results indicate that the realization of a catalytically effective pattern requires the three‐electron reduction of (dpp‐bian)NiBr2. The chemically reduced complexes [K(THF)6]+[(dpp‐bian)Ni(COD)]– and [K(THF)6]+[(dpp‐bian)2Ni]– were synthesized and structurally characterized. Analyzing the data from the electron paramagnetic resonance study of the complexes in a solution, along with quantum‐chemical calculations, reveals that the spin density is predominantly localized at their metal centers. The superposition of trajectory maps of the electron density gradient field and the one‐electron electrostatic force field, along with the atomic charges, discloses that, within the first coordination sphere, the interatomic charge transfer occurs from the metal atom to the ligand atoms and that the complex anions can thus be formally described by the general formulas (dpp‐bian)2–Ni+(COD) and (dpp‐bian)2–Ni+. It was shown that the reduced nickel complexes can be oxidized by formic acid; resulting from this reaction, the two‐electron and two‐proton addition product dpp‐bian‐2H is formed.
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