Selective oxidation to synthesize nitriles is critical
for feedstock
manufacturing in the chemical industry. Current strategies typically
involve substitutions of alkyl halides with toxic cyanides or the
use of strong oxidation reagents (oxygen or peroxide) under ammoxidation/oxidation
conditions, setting considerable challenges in energy efficiency,
sustainability, and production safety. Herein, we demonstrate a facile,
green, and safe electrocatalytic route for selective oxidation of
amines to nitriles under ambient conditions, assisted by the anodic
water oxidation on metal-doped α-Ni(OH)2 (a typical
oxygen evolution reaction catalyst). By controlling the balance between
co-adsorption of the amine molecule and hydroxyls on the catalyst
surface, we demonstrate that Mn doping significantly promotes the
subsequent chemical oxidation of amines, resulting in Faradaic efficiencies
of 96% for nitriles under ≥99% conversion. This anodic oxidation
is further coupled with cathodic hydrogen evolution for overall atomic
economy and additional green energy production.
The selective hydrogenation and rearrangement of 5-hydroxymethylfurfural (5-HMF) to 3-hydroxymethyl-cyclopentone (HCPN) were studied over a MOF-derived bimetallic nickel–copper catalyst in water.
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