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Facile synthesis of controllable graphene-co-shelled reusable Ni/NiO nanoparticles and their application in the synthesis of amines under mild conditions
Liu, Jianguo1,2; Zhu, Yuting1,3; Wang, Chenguang1; Singh, Thishana4; Wang, Nan1,5; Liu, Qiying1; Cui, Zhibing1; Ma, Longlong1,5
2020-11-07
发表期刊GREEN CHEMISTRY
ISSN1463-9262
卷号22期号:21页码:7387-7397
通讯作者Liu, Jianguo(mall@ms.giec.ac.cn) ; Ma, Longlong()
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.
DOI10.1039/d0gc02421j
关键词[WOS]CATALYZED REDUCTIVE AMINATION ; ALKYL-ARYL KETONES ; SELECTIVE CONVERSION ; ASYMMETRIC-SYNTHESIS ; ANTI-MARKOVNIKOV ; CARBON NANOTUBES ; N-METHYLAMINES ; IRON CATALYSTS ; HYDROGENATION ; METHYLATION
收录类别SCI
语种英语
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研究方向Chemistry ; Science & Technology - Other Topics
项目资助者National Natural Science Foundation of China ; National Key R&D Program of China ; DNL Cooperation Fund, CAS
WOS类目Chemistry, Multidisciplinary ; Green & Sustainable Science & Technology
WOS记录号WOS:000583614600011
出版者ROYAL SOC CHEMISTRY
引用统计
被引频次:38[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.giec.ac.cn/handle/344007/34875
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, Guangdong Prov Key Lab New & Renewable Energy Res, CAS Key Lab Renewable Energy, Guangzhou 510640, Peoples R China
2.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
4.Univ KwaZulu Natal, Sch Chem & Phys, Durban 4000, South Africa
5.Tianjin Univ, Sch Environm Sci & Engn, Tianjin 300350, Peoples R China
第一作者单位中国科学院广州能源研究所
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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.
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