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Atomically dispersed Co-N4 sites anchored on N-doped carbon for aqueous phase transfer hydrogenation between nitroarenes and saturated N-heterocycles
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2021-09-03 , DOI: 10.1016/j.apcatb.2021.120681
Dan Xu 1 , Ruirui Liu 1 , Jianfeng Li 1 , Huacheng Zhao 1 , Jiantai Ma 1 , Zhengping Dong 1
Affiliation  

Transfer hydrogenation reactions using non-noble metal-based nanocatalysts are extensively attractive due to their low-cost and green reaction conditions. But construction of such catalysts with maximum metal atom efficiency and high catalytic activity is still a challenging research goal. Here, atomically dispersed Co catalysts with Co-N4 active sites were fabricated, which builds a bridge for transfer hydrogenation between nitroarenes and saturated N-heterocycles in aqueous solution. The TOF value of the transfer hydrogenation reaction is much higher than nanoparticle catalyst for this reaction. Density functional theory (DFT) calculations and control experiments reveal that the excellent performance origins from the Co-N4 sites, which combines the dehydrogenation of 1,2,3,4-tetrahydroquinoline with hydrogenation of nitrobenzene in one-pot. This work not only has an in-depth understanding of active sites but also shows a unique activity to the challenging, highly efficient, and green transfer hydrogenation reaction.



中文翻译:

原子分散的 Co-N4 位点锚定在 N 掺杂的碳上,用于硝基芳烃和饱和 N-杂环之间的水相转移氢化

使用非贵金属基纳米催化剂的转移氢化反应由于其低成本和绿色反应条件而具有广泛的吸引力。但是构建具有最大金属原子效率和高催化活性的催化剂仍然是一个具有挑战性的研究目标。在这里,制备了具有 Co-N 4活性位点的原子分散 Co 催化剂,它为水溶液中硝基芳烃和饱和 N-杂环之间的转移氢化建立了桥梁。转移氢化反应的TOF值远高于该反应的纳米颗粒催化剂。密度泛函理论 (DFT) 计算和控制实验表明,优异的性能源于 Co-N 4位点,将 1,2,3,4-四氢喹啉的脱氢与硝基苯的加氢在一锅法中相结合。这项工作不仅对活性位点有深入的了解,而且对具有挑战性的、高效的、绿色的转移氢化反应也显示出独特的活性。

更新日期:2021-09-15
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