Facile synthesis of controllable graphene-co-shelled reusable Ni/NiO nanoparticles and their application in the synthesis of amines under mild conditions

doi:10.1039/d0gc02421j

	Facile synthesis of controllable graphene-co-shelled reusable Ni/NiO nanoparticles and their application in the synthesis of amines under mild conditions
	Liu, Jianguo 4,5; Zhu, Yuting 3,5; Wang, Chenguang 5; Singh, Thishana 2; Wang, Nan 1,5; Liu, Qiying 5; Cui, Zhibing 5; Ma, Longlong 1,5
刊名	GREEN CHEMISTRY
	2020-11-07
卷号	22 期号:21 页码:7387-7397
ISSN号	1463-9262
DOI	10.1039/d0gc02421j
通讯作者	Liu, Jianguo(mall@ms.giec.ac.cn) ; Ma, Longlong()
英文摘要	The primary objective of many researchers in chemical synthesis is the development of recyclable and easily accessible catalysts. These catalysts should preferably be made from Earth-abundant metals and have the ability to be utilised in the synthesis of pharmaceutically important compounds. Amines are classified as privileged compounds, and are used extensively in the fine and bulk chemical industries, as well as in pharmaceutical and materials research. In many laboratories and in industry, transition metal catalysed reductive amination of carbonyl compounds is performed using predominantly ammonia and H-2. However, these reactions usually require precious metal-based catalysts or RANEY (R) nickel, and require harsh reaction conditions and yield low selectivity for the desired products. Herein, we describe a simple and environmentally friendly method for the preparation of thin graphene spheres that encapsulate uniform Ni/NiO nanoalloy catalysts (Ni/NiO@C) using nickel citrate as the precursor. The resulting catalysts are stable and reusable and were successfully used for the synthesis of primary, secondary, tertiary, and N-methylamines (more than 62 examples). The reaction couples easily accessible carbonyl compounds (aldehydes and ketones) with ammonia, amines, and H-2 under very mild industrially viable and scalable conditions (80 degrees C and 1 MPa H-2 pressure, 4 h), offering cost-effective access to numerous functionalized, structurally diverse linear and branched benzylic, heterocyclic, and aliphatic amines including drugs and steroid derivatives. We have also demonstrated the scale-up of the heterogeneous amination protocol to gram-scale synthesis. Furthermore, the catalyst can be immobilized on a magnetic stirring bar and be conveniently recycled up to five times without any significant loss of catalytic activity and selectivity for the product.
资助项目	National Natural Science Foundation of China[51976225] ; National Key R&D Program of China[2018YFB1501502] ; DNL Cooperation Fund, CAS[DNL201916]
WOS关键词	CATALYZED REDUCTIVE AMINATION ; ALKYL-ARYL KETONES ; SELECTIVE CONVERSION ; ASYMMETRIC-SYNTHESIS ; ANTI-MARKOVNIKOV ; CARBON NANOTUBES ; N-METHYLAMINES ; IRON CATALYSTS ; HYDROGENATION ; METHYLATION
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:000583614600011
资助机构	National Natural Science Foundation of China ; National Key R&D Program of China ; DNL Cooperation Fund, CAS
内容类型	期刊论文
源URL	[http://ir.giec.ac.cn/handle/344007/34874]
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.Tianjin Univ, Sch Environm Sci & Engn, Tianjin 300350, Peoples R China 2.Univ KwaZulu Natal, Sch Chem & Phys, Durban 4000, South Africa 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 5.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangdong Prov Key Lab New & Renewable Energy Res, CAS Key Lab Renewable Energy, Guangzhou 510640, Peoples R China
推荐引用方式 GB/T 7714	Liu, Jianguo,Zhu, Yuting,Wang, Chenguang,et al. Facile synthesis of controllable graphene-co-shelled reusable Ni/NiO nanoparticles and their application in the synthesis of amines under mild conditions[J]. GREEN CHEMISTRY,2020,22(21):7387-7397.
APA	Liu, Jianguo.,Zhu, Yuting.,Wang, Chenguang.,Singh, Thishana.,Wang, Nan.,...&Ma, Longlong.(2020).Facile synthesis of controllable graphene-co-shelled reusable Ni/NiO nanoparticles and their application in the synthesis of amines under mild conditions.GREEN CHEMISTRY,22(21),7387-7397.
MLA	Liu, Jianguo,et al."Facile synthesis of controllable graphene-co-shelled reusable Ni/NiO nanoparticles and their application in the synthesis of amines under mild conditions".GREEN CHEMISTRY 22.21(2020):7387-7397.