Acid Properties of Nanocarbons and Their Application in Oxidative Dehydrogenation

doi:10.1021/acscatal.5b00307

IMR OpenIR

	Acid Properties of Nanocarbons and Their Application in Oxidative Dehydrogenation
	Wen, Guodong 1; Diao, Jiangong 1,2; Wu, Shuchang 1; Yang, Weimin 3; Schoegl, Robert 4; Su, Dang Sheng 1
通讯作者	Su, Dang Sheng(dssu@imr.ac.cn)
	2015-06-01
发表期刊	ACS CATALYSIS
ISSN	2155-5435
卷号	5 期号:6 页码:3600-3608
摘要	Carbon is emerging as an important metal-free catalyst for multiple types of heterogeneous catalysis, including thermocatalysis, photocatalysis, and electrocatalysis. However, the study of mechanisms for carbon catalysis has been impeded at an early stage due to the lack of quantitative research, especially the intrinsic kinetics (e.g., intrinsic TOF). In many carbon-catalyzed reactions, the surface oxygenated groups were found to be the active sites. Recently, we have shown that these oxygenated groups could be identified and quantified via poisoning by small organic molecules; however, these small molecules were toxic. As most of the oxygenated groups are acidic groups, they could also be identified and quantified with respect to the acid properties. More importantly, the method based on acid properties is very green and environmentally benign, because only inorganic bases are added. In this work, the acid properties of carbon nanotubes (CNTs) treated by concentrated HNO3 were thoroughly studied by mass titration and Boehm titration. The two titration methods were also compared to the conventional methods for acidity analysis including NH3 pulse adsorption, NH3-TPD, and FT-IR. Boehm titration was very effective to quantify the carboxylic acid, lactone, phenol, and carbonyl groups, and the findings were consistent with the results from XPS and NH3 pulse adsorption. These CNTs were applied in the oxidative dehydrogenation (ODH) of ethylbenzene, and the activity of these catalysts exhibited a good linear dependence on the number of carbonyl groups. The value of TOF for the carbonyl group obtained from Boehm titration was 3.2 x 10(-4) s(-1) (245 degrees C, atmosphere pressure, 2.8 kPa ethylbenzene, 5.3 kPa O-2). For better understanding the acidity of nanocarbon, these CNTs were also applied in two acid-catalyzed reactions (Beckmann rearrangement and ring opening), and a good linear relationship between the conversion and the number of acidic sites was found.
关键词	acid properties nanocarbon oxidative dehydrogenation mass titration Boehm titration
资助者	Ministry of Science and Technology of China ; National Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Doctoral Starting up Foundation of Liaoning Province, China
DOI	10.1021/acscatal.5b00307
收录类别	SCI
语种	英语
资助项目	Ministry of Science and Technology of China[2011CBA00504] ; National Science Foundation of China[21133010] ; National Science Foundation of China[51221264] ; National Science Foundation of China[21261160487] ; National Science Foundation of China[21411130120] ; National Science Foundation of China[21473223] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDA09030103] ; Doctoral Starting up Foundation of Liaoning Province, China[20121068]
WOS研究方向	Chemistry
WOS类目	Chemistry, Physical
WOS记录号	WOS:000355964300046
出版者	AMER CHEMICAL SOC
引用统计
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/81196
通讯作者	Su, Dang Sheng
作者单位	1.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Peoples R China 2.Grad Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Shanghai Res Inst Petrochem Technol, Shanghai 201208, Peoples R China 4.Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, D-14195 Berlin, Germany
推荐引用方式 GB/T 7714	Wen, Guodong,Diao, Jiangong,Wu, Shuchang,et al. Acid Properties of Nanocarbons and Their Application in Oxidative Dehydrogenation[J]. ACS CATALYSIS,2015,5(6):3600-3608.
APA	Wen, Guodong,Diao, Jiangong,Wu, Shuchang,Yang, Weimin,Schoegl, Robert,&Su, Dang Sheng.(2015).Acid Properties of Nanocarbons and Their Application in Oxidative Dehydrogenation.ACS CATALYSIS,5(6),3600-3608.
MLA	Wen, Guodong,et al."Acid Properties of Nanocarbons and Their Application in Oxidative Dehydrogenation".ACS CATALYSIS 5.6(2015):3600-3608.