IMR OpenIR
Structure-performance relationship of nanodiamonds @ nitrogen-doped mesoporous carbon in the direct dehydrogenation of ethylbenzene
Liu, YF; Ba, H; Luo, JJ; Wu, KH; Nhut, JM; Su, DS; Pham-Huu, C; Su, DS (reprint author), Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy DNL, 457 Zhongshan Rd, Dalian 116023, Peoples R China.; Pham-Huu, C (reprint author), Univ Strasbourg, CNRS, UMR 7515, ICPEES,ECPM, 25 Rue Becquerel, F-67087 Strasbourg 02, France.
2018-03-01
发表期刊CATALYSIS TODAY
ISSN0920-5861
卷号301页码:38-47
摘要Nanocarbon materials have been reported as an alternative robust metal-free catalyst in the field of the catalytic dehydrogenation with improved catalytic performance as well as stability. In this study, the hybrid metal-free catalyst consisting of dispersed nanodiamonds within a nitrogen-doped mesoporous carbon (ND@NMC) phase was investigated. Such material with high effective surface area and porosity was prepared under different thermal treatment temperatures and further evaluated for the direct dehydrogenation (DDH) of ethylbenzene (EB) to styrene (ST). The characterization techniques such as N-2 adsorption-desorption, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy and Raman spectroscopic analysis were used to investigate the surface properties and structures of the as-prepared ND@NMC composites. The ND@NMC-700 catalyst annealed at 700 degrees C presented a ST specific reaction rate and a relative areal activity of 5.8 mmolST g(catalyst)(-1) h(-1) and 0.28 mu mol(ST) m(-2) h(-1) with a ST selectivity of 99.6%, which is the highest DDH activity among the investigated nanocarbons including ND, carbon nanotubes, NMC and ND@MC (ND covered by mesoporous carbon) catalysts. The superior dehydrogenation performance could be attributed to the high dispersion of the metal-free nanodiamond centers within the NMC layer which provided a well surface contact with the reactant. It can also be confirmed that the rational contents of ketone (C = O) functional groups, as well as the opened porous network in ND@NMC-700 catalyst resulted to the superior DDH activity and styrene selectivity. Moreover, the presented nitrogen groups are beneficial for construction of surface defects and porosity as well as the improvement of styrene selectivity.; Nanocarbon materials have been reported as an alternative robust metal-free catalyst in the field of the catalytic dehydrogenation with improved catalytic performance as well as stability. In this study, the hybrid metal-free catalyst consisting of dispersed nanodiamonds within a nitrogen-doped mesoporous carbon (ND@NMC) phase was investigated. Such material with high effective surface area and porosity was prepared under different thermal treatment temperatures and further evaluated for the direct dehydrogenation (DDH) of ethylbenzene (EB) to styrene (ST). The characterization techniques such as N-2 adsorption-desorption, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy and Raman spectroscopic analysis were used to investigate the surface properties and structures of the as-prepared ND@NMC composites. The ND@NMC-700 catalyst annealed at 700 degrees C presented a ST specific reaction rate and a relative areal activity of 5.8 mmolST g(catalyst)(-1) h(-1) and 0.28 mu mol(ST) m(-2) h(-1) with a ST selectivity of 99.6%, which is the highest DDH activity among the investigated nanocarbons including ND, carbon nanotubes, NMC and ND@MC (ND covered by mesoporous carbon) catalysts. The superior dehydrogenation performance could be attributed to the high dispersion of the metal-free nanodiamond centers within the NMC layer which provided a well surface contact with the reactant. It can also be confirmed that the rational contents of ketone (C = O) functional groups, as well as the opened porous network in ND@NMC-700 catalyst resulted to the superior DDH activity and styrene selectivity. Moreover, the presented nitrogen groups are beneficial for construction of surface defects and porosity as well as the improvement of styrene selectivity.
部门归属[liu, yuefeng ; su, dang sheng] chinese acad sci, dalian inst chem phys, dalian natl lab clean energy dnl, 457 zhongshan rd, dalian 116023, peoples r china ; [liu, yuefeng ; ba, housseinou ; nhut, jean-mario ; pham-huu, cuong] univ strasbourg, cnrs, umr 7515, icpees,ecpm, 25 rue becquerel, f-67087 strasbourg 02, france ; [luo, jingjie ; wu, kuang-hsu ; su, dang sheng] chinese acad sci, inst met res, shenyang natl lab mat sci, 72 wenhua rd, shenyang 110016, liaoning, peoples r china
关键词Metal-free Catalyst Steam-free Dehydrogenation Styrene Production Oxygen Reduction Oxidative Dehydrogenation Surface-chemistry Functional-groups Nanotubes Nanocarbon Composite
学科领域Chemistry, Applied ; Chemistry, Physical ; Engineering, Chemical
资助者NSFC of China [21473223, 21606243, 91645117]; FREECATS project - European Union within 7FP research program [NMP3-SL-2012-280658]; China Postdoctoral Science Foundation [2016M600221]
收录类别SCI
语种英语
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/79482
专题中国科学院金属研究所
通讯作者Liu, YF; Su, DS (reprint author), Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy DNL, 457 Zhongshan Rd, Dalian 116023, Peoples R China.; Pham-Huu, C (reprint author), Univ Strasbourg, CNRS, UMR 7515, ICPEES,ECPM, 25 Rue Becquerel, F-67087 Strasbourg 02, France.
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GB/T 7714
Liu, YF,Ba, H,Luo, JJ,et al. Structure-performance relationship of nanodiamonds @ nitrogen-doped mesoporous carbon in the direct dehydrogenation of ethylbenzene[J]. CATALYSIS TODAY,2018,301:38-47.
APA Liu, YF.,Ba, H.,Luo, JJ.,Wu, KH.,Nhut, JM.,...&Pham-Huu, C .(2018).Structure-performance relationship of nanodiamonds @ nitrogen-doped mesoporous carbon in the direct dehydrogenation of ethylbenzene.CATALYSIS TODAY,301,38-47.
MLA Liu, YF,et al."Structure-performance relationship of nanodiamonds @ nitrogen-doped mesoporous carbon in the direct dehydrogenation of ethylbenzene".CATALYSIS TODAY 301(2018):38-47.
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