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Biomass Sucrose‐Derived Cobalt@Nitrogen‐Doped Carbon for Catalytic Transfer Hydrogenation of Nitroarenes with Formic Acid
ChemSusChem ( IF 7.5 ) Pub Date : 2018-10-26 , DOI: 10.1002/cssc.201802163
Man Yuan 1 , Yu Long 1 , Jin Yang 1 , Xiwei Hu 1 , Dan Xu 1 , Yangyang Zhu 1 , Zhengping Dong 1
Affiliation  

Fabrication of non‐noble metal‐based heterogeneous catalysts by a facile and cost‐effective strategy for ecofriendly catalytic transfer hydrogenation (CTH) is of great significance for organic transformations. A cobalt@nitrogen‐doped carbon (Co@NC) catalyst was prepared from renewable biomass‐derived sucrose, harmless melamine, and earth‐abundant Co(AcO)2 as the precursor materials by hydrothermal treatment and carbonization. Co nanoparticles (NPs) were coated with NC shells and uniformly embedded in the NC framework. The as‐obtained Co@NC‐600 (carbonized at 600 °C) catalyst exhibited excellent catalytic efficiency for CTH of various functionalized nitroarenes with formic acid (FA) as hydrogen donor in aqueous solution. The uniformly incorporated N atoms in the C matrix and the encapsulated Co NPs showed synergistic effects in the CTH reactions. A mechanistic analysis indicated that the protons from FA were activated by Co sites after being captured by N atoms, and then reacted with nitroarenes adsorbed on the surface of the catalysts to generate the corresponding aromatic amines. Moreover, the catalyst showed excellent durability and reusability without obvious decrease in activity even after five reaction cycles. Thus, the study reported herein provides a cost‐effective, sustainable strategy for fabrication of biomass‐derived non‐noble metal‐based catalysts for green and efficient catalytic transformations.

中文翻译:

生物质蔗糖衍生的钴@氮掺杂碳,用于甲酸对硝基芳烃的催化转移加氢

通过一种简便且具有成本效益的生态友好型催化转移加氢(CTH)策略制造非贵金属基多相催化剂对于有机转化具有重要意义。用可再生生物质衍生的蔗糖,无害的三聚氰胺和富含地球的Co(AcO)2制备了钴氮掺杂碳(Co @ NC)催化剂。作为前体材料经水热处理和碳化。Co纳米颗粒(NPs)涂有NC壳层,并均匀地嵌入NC框架中。如此制得的Co @ NC-600(在600°C碳化)催化剂对各种功能化硝基芳烃的CTH表现出优异的催化效率,其中甲酸(FA)为水溶液中的氢供体。在C基质中均匀掺入的N原子和被包封的Co NP在CTH反应中显示出协同作用。机理分析表明,来自FA的质子在被N原子捕获后被Co位活化,然后与吸附在催化剂表面的硝基芳烃反应生成相应的芳族胺。而且,该催化剂即使在五个反应循环后仍显示出优异的耐久性和可重复使用性,而活性没有明显降低。因此,本文报道的研究为生物质衍生的非贵金属基催化剂的制造提供了一种经济高效的可持续策略,以实现绿色高效的催化转化。
更新日期:2018-10-26
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