脱氢
催化作用
钴
碳纤维
氮气
多孔性
材料科学
醛
化学
无机化学
有机化学
化学工程
复合数
复合材料
工程类
作者
Cheng Chen,Zhiqin Wang,Yanyan Gong,Jichao Wang,Ye Yuan,Hua Cheng,Wei Sang,Somboon Chaemchuen,Francis Verpoort
出处
期刊:Carbon
[Elsevier BV]
日期:2021-04-01
卷期号:174: 284-294
被引量:27
标识
DOI:10.1016/j.carbon.2020.12.040
摘要
Herein, cobalt embedded in nitrogen-doped porous carbon ([email protected]) was developed as a robust heterogeneous catalyst for the dehydrogenative coupling of primary alcohols and hydroxides. With [email protected] as the first earth-abundant metal/carbon composite material for this transformation, numerous aromatic and aliphatic carboxylic acids were efficiently afforded. Notably, the newly prepared [email protected] was fabricated in a facile and straightforward manner and reused up to 15 recycle rounds without activity decay. It is also worth emphasizing that the catalyst recycling was realized via magnetic separation with no special treatment or activation. Additionally, further experiments elucidated the pivotal role of the cobalt and nitrogen elements dispersed in the carbon matrix as well as the hierarchical porosity (micro-/meso-pores) in the catalytic activity and recyclability. Considering the active sites of [email protected], we envisioned that the Co–N species was the most active site, while other active sites such as Co–O, Co0 species and free N-doped carbon were also present, but demonstrating lower activity or stability in comparison with the Co–N species. Additional mechanistic investigations were carried out to gain more insights into the possible reaction pathways. We found that the aldehyde was identified as a crucial intermediate, and two possible pathways were proposed for this catalytic process.
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