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A Dinuclear Nickel Complex for Electrocatalytic Nitrite Reduction.

Sheyda Partovi1, Yaroslav Losovyj1,2, Nobuyuki Yamamoto1

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Dinuclear nickel complexes offer new avenues for nitrite electroreduction. The dinuclear complex [Ni2(tpmc)(NO3)2]2+ shows improved catalytic onset potential compared to its mononuclear counterpart, producing ammonium.

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Area of Science:

  • Coordination Chemistry
  • Electrocatalysis
  • Inorganic Chemistry

Background:

  • Mononuclear complexes are widely studied for electrocatalytic nitrite reduction.
  • Dinuclear electrocatalysts for nitrite reduction are less explored.
  • Understanding the role of metal-metal interactions in catalysis is crucial.

Purpose of the Study:

  • To investigate the electrocatalytic nitrite reduction by a novel dinuclear nickel complex, [Ni2(tpmc)(NO3)2]2+.
  • To compare its performance with a mononuclear analogue, [Ni(cyclam)]2+.
  • To elucidate the effect of dinuclearity on catalytic activity and product selectivity.

Main Methods:

  • Electrochemical synthesis and characterization of dinuclear and mononuclear nickel complexes.
  • Cyclic voltammetry and rotating disk electrode studies for electrocatalytic activity.
  • Product analysis using spectroscopic methods to determine Faradaic efficiency.

Main Results:

  • The dinuclear complex [Ni2(tpmc)(NO3)2]2+ exhibited an anodic shift in the onset potential for nitrite reduction by approximately 0.3 V compared to [Ni(cyclam)]2+.
  • Both complexes demonstrated comparable electrocatalytic rates and Faradaic efficiencies for ammonium production.
  • Aqueous Ni2+ ions showed faster catalysis at a more anodic potential than [Ni(cyclam)]2+, albeit with lower Faradaic efficiency.

Conclusions:

  • Dinuclear nickel complexes can enhance electrocatalytic nitrite reduction by shifting the onset potential anodically.
  • The presence of a second metal ion influences the catalytic properties without significantly altering the primary reduction product (ammonium).
  • Further research into dinuclear systems could lead to more efficient electrocatalysts for nitrogen compound transformations.