Structure-performance relationship of nanodiamonds @ nitrogen-doped mesoporous carbon in the direct dehydrogenation of ethylbenzene

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
ISSN	0920-5861
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
WOS记录号	WOS:000417054300007
引用统计	被引频次：36[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/321006/79482
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.
推荐引用方式 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.