Atomically dispersed cobalt catalysts for tandem synthesis of primary benzylamines from oxidized β-O-4 segments

• Published in: Chemical science (Cambridge) Vol. 15; no. 28; pp. 1954 - 1962
• Main Authors: Luan, Sen, Wu, Wei, Zheng, Bingxiao, Wu, Yuxuan, Dong, Minghua, Shen, Xiaojun, Wang, Tianjiao, Deng, Zijie, Zhang, Bin, Chen, Bingfeng, Xing, Xueqing, Wu, Haihong, Liu, Huizhen, Han, Buxing
• Format: Journal Article
• Language: English
• Published: CAMBRIDGE Royal Soc Chemistry 17.07.2024; Royal Society of Chemistry; The Royal Society of Chemistry
• Subjects: Cascade chemical reactions; Catalysts; Chemical synthesis; Chemistry; Chemistry, Multidisciplinary; Cobalt compounds; Coordination numbers; Hydrogenolysis; Lignin; Nitrogen; Physical Sciences; Science & Technology; OXIDATION; TRANSFORMATION; AMINATION; HETEROCYCLES; METAL-CATALYSTS; CONVERSION; CHEMICALS; COORDINATION; LIGNOCELLULOSE; LIGNIN
• ISSN: 2041-6520; 2041-6539
• DOI: 10.1039/d4sc01813c

This work presents an innovative approach focusing on fine-tuning the coordination environment of atomically dispersed cobalt catalysts for tandem synthesis of primary benzylamines from oxidized lignin model compounds. By meticulously regulating the Co-N coordination environment, the activity of these catalysts in the hydrogenolysis and reductive amination reactions was effectively controlled. Notably, our study demonstrates that, in contrast to cobalt nanoparticle catalysts, atomically dispersed cobalt catalysts exhibit precise control of the sequence of hydrogenolysis and reductive amination reactions. Particularly, the CoN3 catalyst with a triple Co-N coordination number achieved a remarkable 94% yield in the synthesis of primary benzylamine. To our knowledge, there is no previous documentation of the synthesis of primary benzylamines from lignin dimer model compounds. Our study highlights a promising one-pot route for sustainable production of nitrogen-containing aromatic chemicals from lignin. This research investigates fine-tuning single-atom cobalt catalysts for conversion of oxidized lignin model compounds to benzylamines through a controlled hydrogenolysis and reductive amination tandem reaction.