Simplified preparation of a graphene-co-shelled Ni/NiO@C nano-catalyst and its application in the N-dimethylation synthesis of amines under mild conditions

doi:10.1039/d1gc00981h

	Simplified preparation of a graphene-co-shelled Ni/NiO@C nano-catalyst and its application in the N-dimethylation synthesis of amines under mild conditions
	Liu, Jianguo 1,3; Song, Yanpei 1,2; Zhuang, Xiuzheng 1,2; Zhang, Mingyue 1,2; Ma, Longlong 1
刊名	GREEN CHEMISTRY
	2021-06-04
页码	14
ISSN号	1463-9262
DOI	10.1039/d1gc00981h
通讯作者	Liu, Jianguo(liujg@ms.giec.ac.cn) ; Ma, Longlong(mall@ms.giec.ac.cn)
英文摘要	The development of Earth-abundant, reusable and non-toxic heterogeneous catalysts to be applied in the pharmaceutical industry for bio-active relevant compound synthesis remains an important goal of general chemical research. N-methylated compounds, as one of the most essential bioactive compounds, have been widely used in the fine and bulk chemical industries for the production of high-value chemicals. Herein, an environmentally friendly and simplified method for the preparation of graphene encapsulated Ni/NiO nanoalloy catalysts (Ni/NiO@C) was developed for the first time, for the highly selective synthesis of N-methylated compounds using various functional amines and aldehydes under easy to handle, and industrially applicable conditions. A large number of primary and secondary amines (more than 70 examples) could be converted to the corresponding N,N-dimethylamines with the participation of different functional aldehydes, with an average yield of over 95%. A gram-scale synthesis also demonstrated a similar yield when compared with the benchmark test. In addition, it was further proved that the catalyst could easily be recycled because of its intrinsic magnetism and reused up to 10 times without losing its activity and selectivity. Also, for the first time, the tandem synthesis of N,N-dimethylamine products in a one-pot process, using only a single earth-abundant metal catalyst, whose activity and selectivity were more than 99% and 94%, respectively, for all tested substrates, was developed. Overall, the advantages of this newly developed method include operational simplicity, high stability, easy recyclability, cost-effectiveness of the catalyst, and good functional group compatibility for the synthesis of N-methylation products as well as the industrially applicable tandem synthesis process.
资助项目	National Key R&D Program of China[2018YFB1501500] ; National Natural Science Foundation of China[51976225] ; DNL Cooperation Fund ; Chinese Academy of Sciences[DNL201916]
WOS关键词	CARBON-DIOXIDE ; REDUCTIVE METHYLATION ; AROMATIC-AMINES ; NITRO-COMPOUNDS ; CHEMOSELECTIVE METHYLATION ; GENERAL-SYNTHESIS ; SECONDARY-AMINES ; FORMIC-ACID ; EFFICIENT ; HYDROGENATION
WOS研究方向	Chemistry ; Science & Technology - Other Topics
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000660120300001
资助机构	National Key R&D Program of China ; National Natural Science Foundation of China ; DNL Cooperation Fund ; Chinese Academy of Sciences
内容类型	期刊论文
源URL	[http://ir.giec.ac.cn/handle/344007/33337]
专题	中国科学院广州能源研究所
通讯作者	Liu, Jianguo; Ma, Longlong
作者单位	1.Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou 510640, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Liu, Jianguo,Song, Yanpei,Zhuang, Xiuzheng,et al. Simplified preparation of a graphene-co-shelled Ni/NiO@C nano-catalyst and its application in the N-dimethylation synthesis of amines under mild conditions[J]. GREEN CHEMISTRY,2021:14.
APA	Liu, Jianguo,Song, Yanpei,Zhuang, Xiuzheng,Zhang, Mingyue,&Ma, Longlong.(2021).Simplified preparation of a graphene-co-shelled Ni/NiO@C nano-catalyst and its application in the N-dimethylation synthesis of amines under mild conditions.GREEN CHEMISTRY,14.
MLA	Liu, Jianguo,et al."Simplified preparation of a graphene-co-shelled Ni/NiO@C nano-catalyst and its application in the N-dimethylation synthesis of amines under mild conditions".GREEN CHEMISTRY (2021):14.