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Preparation of Ni/C Core-shell Nanoparticles through MOF Pyrolysis for Phenylacetylene Hydrogenation Reaction
Guo Xiaoling1,2; Chen Xiao1; Su Dangsheng2; Liang Changhai1
通讯作者Liang Changhai(changhai@dlut.edu.cn)
2018
发表期刊ACTA CHIMICA SINICA
ISSN0567-7351
卷号76期号:1页码:22-29
摘要A series of Ni/C core-shell nano catalysts with abundant mesoporous and uniform size were prepared by Ni-MOF-74 pyrolysis. The Ni-MOF-74 was synthesized via hydrothermal method with nickel acetate and 2,5-dihydroxyterephthalic acid (DHTA) as raw materials. The pyrolysis process was carried out in a tube furnace under Argon (Ar) atmosphere with a heating rate of 2 degrees C/min. Completed pyrolytic product Ni/C can be obtained by extending the pyrolysis time (6 h) at 400. or increasing the pyrolysis temperature (>= 500 degrees C) based on the TG result. Moreover, the particle size of Ni/C varied with pyrolysis temperature from 3 nm (500 degrees C) to 17 nm (800 degrees C). The TEM images and Ar ion sputtering XPS indicated a core-shell structure of the pyrolysis product. Nickel species can be stable in the form of nickel (Ni-0) due to the electronic properties regulating and confinement effect of the carbon shell. Moreover, the carbon shell greatly weaken the interaction between particles, which is favorable for the dispersion of the catalyst in the reaction system. H-2-TPR results show that the interaction between nickel and amorphous carbon increases with the pyrolysis temperature, which is unfavorable to the interaction between Ni species and the reactant. The phenylacetylene (PA) hydrogenation reaction was carried out with 0.2 g catalyst, 10 mL of 1 mol/L ethanolic phenylacetylene solution and 1.0 MPa H-2 in a 50 mL high-pressure autoclave under 50 degrees C. Ni/C exhibits excellent catalytic activity and recyclability in phenylacetylene (PA) hydrogenation. In addition, we compared the activity of Ni/C with several reported catalyst system and found their activity increases in the order of Ni, NiSix, supported Ni2Si, Ni/C, Pd and Pt. With an activity of up to 0.833 mmol.min(-1).g(cat).(-1) at 50 degrees C (Ni/C-400-6, Ni/C-500-2), Ni/C is the most promising transition metal catalyst that can be comparable with noble metal.
关键词MOFs pyrolysis Ni/C nano-material core-shell structure heterogeneous catalysis phenylacetylene hydrogenation
资助者National Natural Science Foundation of China ; Natural Science Foundation of Liaoning Province in China ; Fundamental Research Funds for the Central Universities
DOI10.6023/A17070339
收录类别SCI
语种英语
资助项目National Natural Science Foundation of China[21373038] ; National Natural Science Foundation of China[21403026] ; Natural Science Foundation of Liaoning Province in China[2015021014] ; Fundamental Research Funds for the Central Universities[DUT16RC(4)03]
WOS研究方向Chemistry
WOS类目Chemistry, Multidisciplinary
WOS记录号WOS:000428734300002
出版者SCIENCE PRESS
引用统计
被引频次:18[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/127718
专题中国科学院金属研究所
通讯作者Liang Changhai
作者单位1.Dalian Univ Technol, Sch Chem Engn, Lab Adv Mat & Catalyt Engn, Dalian 116024, Peoples R China
2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China
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Guo Xiaoling,Chen Xiao,Su Dangsheng,et al. Preparation of Ni/C Core-shell Nanoparticles through MOF Pyrolysis for Phenylacetylene Hydrogenation Reaction[J]. ACTA CHIMICA SINICA,2018,76(1):22-29.
APA Guo Xiaoling,Chen Xiao,Su Dangsheng,&Liang Changhai.(2018).Preparation of Ni/C Core-shell Nanoparticles through MOF Pyrolysis for Phenylacetylene Hydrogenation Reaction.ACTA CHIMICA SINICA,76(1),22-29.
MLA Guo Xiaoling,et al."Preparation of Ni/C Core-shell Nanoparticles through MOF Pyrolysis for Phenylacetylene Hydrogenation Reaction".ACTA CHIMICA SINICA 76.1(2018):22-29.
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