Shu‐Lin Meng, Wenjie Kang, Chen-Ho Tung, Li-Zhu Wu
As an important category of organic nitrogenous compounds, oxime synthesis requires extensive energy input to fulfill multielectron transformation. Herein, we accomplish oxime synthesis via a spontaneous reaction for the first time under ambient conditions. By intimately assembling aluminum (Al) with a NO x – ( x = 2, 3) reduction catalyst, the multielectron oxime synthesis proceeds with excellent yields, in which Al offers a strong driving force and high capacity for electron transfer, and CuZn alloy foil as an efficient catalyst presents extraordinary stability. Using abundant NO x – feedstocks, the C–N coupling is achieved to realize tandem, gram-scale air-to-oxime synthesis integrating plasma-driven N 2 oxidation. Taking advantage of recycled Al resources, the oxime synthesis method demonstrates promising profitability and energy efficiency. The broad scope of aldehyde and ketone substrates enables successful oximation of bioactive and drug molecules, offering convenient access to utilize abundant resources for the synthesis of value-added nitrogenous compounds.