Highly Stable Porous-Carbon-Coated Ni Catalysts for the Reductive Amination of Levulinic Acid via an Unconventional Pathway | |
Department | 苏州研究院 |
Gao G(高广)1; Sun P(孙鹏)1; Li, Yunqin2; Wang, Fang1; Zhao ZL(赵泽伦)1; Qin, Yong2; Li FW(李福伟)1; Li FW(李福伟) | |
The second department | osso国家重点实验室 |
2017 | |
Source Publication | ACS Catalysis |
ISSN | 2155-5435 |
Volume | 7Issue:8Pages:4927-4935 |
Abstract | The catalytic conversions of biomass and its derivatives into fuels and chemicals require active and stable catalysts. Non-noble-metal catalysts typically suffer from deactivation due to the leaching and sintering of the metal species in liquid-phase reactions. In this work, we report a facile synthesis of porous-carbon-coated Ni catalysts supported on carbon nanotubes (CNFx@Ni@CNTs) by atomic layer deposition for the reductive amination of levulinic acid (LA) with amines to pyrrolidones. Under the protection of porous carbon with a moderate thickness, the optimized CNF30@Ni@CNTs catalyst showed a 99% yield of pyrrolidones and recyclability of up to 20 runs without the leaching and sintering of Ni nanoparticles. On the basis of verification experiments and density functional theory calculations, we determined that our Ni-catalyzed reductive amination of LA with amines underwent an unconventional pathway via amides as the first intermediate, followed by tandem cyclization, intramolecular dehydration, and hydrogenation to the desired pyrrolidones. This pathway was completely different from the reported imine-intermediated route in Pt-catalyzed systems. This work provides insights into the design of active and stable heterogeneous catalysts for liquid-phase reactions as well as into switching reaction pathways to realize the replacement of noble metals for the transformation of biobased multifunctional substrates. |
Subject Area | 物理化学与绿色催化 |
DOI | 10.1021/acscatal.7b01786 |
Funding Organization | the Natural Science Foundation of China (21503242;21522309;21633013;21673269);the Suzhou Science and Technology Projects (SYG201518;SYG201519);the Chinese Academy of Sciences |
Indexed By | SCI |
If | 10.614 |
Language | 英语 |
Funding Project | 均相催化研究组 |
compositor | 第一作者单位 |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.licp.cn/handle/362003/22472 |
Collection | 苏州研究院 羰基合成与选择氧化国家重点实验室(OSSO) |
Corresponding Author | Qin, Yong; Li FW(李福伟) |
Affiliation | 1.Chinese Acad Sci, Lanzhou Inst Chem Phys, Suzhou Res Inst, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Gansu, Peoples R China 2.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China |
Recommended Citation GB/T 7714 | Gao G,Sun P,Li, Yunqin,et al. Highly Stable Porous-Carbon-Coated Ni Catalysts for the Reductive Amination of Levulinic Acid via an Unconventional Pathway[J]. ACS Catalysis,2017,7(8):4927-4935. |
APA | Gao G.,Sun P.,Li, Yunqin.,Wang, Fang.,Zhao ZL.,...&李福伟.(2017).Highly Stable Porous-Carbon-Coated Ni Catalysts for the Reductive Amination of Levulinic Acid via an Unconventional Pathway.ACS Catalysis,7(8),4927-4935. |
MLA | Gao G,et al."Highly Stable Porous-Carbon-Coated Ni Catalysts for the Reductive Amination of Levulinic Acid via an Unconventional Pathway".ACS Catalysis 7.8(2017):4927-4935. |
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acscatal.7b01786.pdf(5853KB) | 期刊论文 | 作者接受稿 | 开放获取 | CC BY-NC-SA | View Application Full Text |
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