A Highly Porous Carbon Support Rich in Graphitic-N Stabilizes Copper Nanocatalysts for Efficient Ethanol Dehydrogenation

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• 作者：Peng Zhang ; Qing-Nan Wang ; Prof. Xia Yang ; Prof. Dongqi Wang ; Prof. Wen-Cui Li ; Dr. Yanping Zheng ; Prof. Mingshu Chen and Prof. An-Hui Lu
• 刊名：ChemCatChem
• 出版年：2017
• 出版时间：February 6, 2017
• 年：2017
• 卷：9
• 期：3
• 页码：505-510
• 全文大小：1492K
• ISSN：1867-3899

文摘

The dehydrogenation of bioethanol to acetaldehyde and hydrogen is a sustainable process, owing to the atom-economical transformation and easy separation of the products. However, oxide-supported Cu catalysts show a low selectivity to acetaldehyde because of considerable side reactions caused by their oxygen-rich surfaces. A conventional carbon-supported Cu catalyst shows high selectivity, but is quickly deactivated owing to the migration and agglomeration of copper particles. Here, we have produced a highly porous nitrogen-rich carbon support that contains 6.2 wt % N and can nicely disperse and stabilize Cu nanoparticles (∼6.3 nm). If used for ethanol dehydrogenation, approximately 98 % selectivity to acetaldehyde has been achieved, with excellent anti-agglomeration ability for as long as 500 min. X-ray photoelectron spectroscopy (XPS) data prove that electrons transfer to the Cu particles from the N sites. Theoretical calculations further show that nitrogen sites enhance the adsorption of Cu₂₀ clusters and can stabilize them against coalescence and that graphitic-N sites (approximately 40 % of total N content) are the most significant.