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Origin of copper dissolution under electrocatalytic reduction conditions involving amines

https://doi.org/10.1039/d4sc01944j

Guan, Yani; Kümper, Justus; Mürtz, Sonja D; Kumari, Simran; Hausoul, Peter_J C; Palkovits, Regina; Sautet, Philippe (September 2024, Chemical Science)

Copper electrodes corrode using mixtures of acetone and methylamine even under reductive potential conditions. Simulations explain this dynamical process from a microscopic perspective through the formation of a surface Cu–amine complex.
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Probing the Electric Double-Layer Capacitance to Understand the Reaction Environment in Conditions of Electrochemical Amination of Acetone

https://doi.org/10.1021/acsami.4c14134

Guan, Yani; Kümper, Justus; Kumari, Simran; Heiming, Nick; Mürtz, Sonja_D; Steinmann, Stephan_N; Palkovits, Stefan; Palkovits, Regina; Sautet, Philippe (January 2025, ACS Applied Materials & Interfaces)
Metallic Impurities in Electrolysis: Catalytic Effect of Pb Traces in Reductive Amination and Acetone Reduction

https://doi.org/10.1002/anie.202411532

Kümper, Justus; Mürtz, Sonja_D; Guan, Yani; Kumari, Simran; Hausoul, Peter_J_C; Kurig, Nils; Sautet, Philippe; Palkovits, Regina (November 2024, Angewandte Chemie International Edition)

Abstract The electrochemical hydrogenation (e‐hydrogenation) of unsaturated compounds like imines or carbonyls presents a benign reduction method. It enables direct use of electrons as reducing agent, water as proton source, while bypassing the need for elevated temperatures or pressures. In this contribution, we discuss the active species in electrocatalytic reductive amination with the transformation of acetone and methylamine as model reaction. Surprisingly, lead impurities in the ppm‐range proved to possess a significant effect in e‐hydrogenation. Accordingly, the influence of applied potential and cathode material in presence of 1 ppm Pb was investigated. Finally, we transferred the insights to the reduction of acetone manifesting comparable observations as for imine reduction. The results suggest that previous studies on electrochemical reduction in the presence of lead electrodes should be re‐evaluated.
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