Ambient One‐Pot Electrocatalytic Synthesis of Caprolactam From Cyclohexanone and Nitrate Over Ag‐Ag <sub>4</sub> Sn‐SnO <sub>2</sub> Nanoparticles
Abstract
ABSTRACT Caprolactam (CPL), a monomer of nylon‐6 widely used in automotive, machinery, and electronics, is traditionally synthesized from cyclohexanone (CYC) through a complex process that generates low‐value ammonium sulfate, leading to environmental pollution. In contrast, electrochemical methods offer a safer, greener one‐pot synthesis of CPL from waste NO 3 – , but currently, the coupling of CYC and NO 3 – primarily produces cyclohexanone oxime (CHO), and the direct generation of CPL is challenging. Here, we report for the first time the electrochemical conversion of CYC and NO 3 – to high‐value CPL in a one‐pot process under ambient conditions. Using Ag‐Ag 4 Sn‐SnO 2 nanoparticle catalysts, we achieved a remarkable 96% yield and 97% selectivity for CPL electrosynthesis. In situ characterizations, control experiments, and theoretical calculations suggested the importance of balanced activation of NO 3 – and CYC substrates on the Ag‐Ag 4 Sn‐SnO 2 catalysts for achieving high‐efficient CPL electrosynthesis. The method also exhibits broad versatility in synthesizing various amide compounds, including paracetamol for antipyretic. Notably, scaling up the reactor enabled a high CPL production rate of 3.41 g h −1 g cat −1 with a 90.5% isolated yield, highlighting the potential of this technique for large‐scale electrosynthesis.
Article Details
Authors (12)
Cheng Xue
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Shuaiqiang Jia
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Xiao Chen
Jiapeng Jiao
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Zhanghui Xia
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Mengke Dong
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Ting Deng
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Hailian Cheng
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Chunjun Chen
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Haihong Wu
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Mingyuan He
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Buxing Han
Institute of Chemistry, Chinese Academy of Sciences , , ,