Nitrogen-doped carbon nanotubes as efficient catalysts for isobutane dehydrogenation

被引:26
作者
Mu, Jiali [1 ]
France, Liam John [1 ]
Liu, Baoan [1 ]
Shi, Junjun [1 ]
Long, Jinxing [1 ]
Lv, LuFeng [2 ]
Li, Xuehui [1 ]
机构
[1] South China Univ Technol, Sch Chem & Chem Engn, Pulp Paper Engn State Key Lab China, Guangzhou 510640, Guangdong, Peoples R China
[2] Sinopec Res Inst Petr Proc, Beijing 100083, Peoples R China
关键词
OXIDATIVE DEHYDROGENATION; SURFACE-CHEMISTRY; GRAPHENE; PROPANE; OXIDE; SPECTROSCOPY; PERFORMANCE; NANOCARBON; BUTADIENE; MELAMINE;
D O I
10.1039/c6cy02314b
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Large-scale production of isobutene from isobutane requires high-performance and cost-effective catalysts. Carbon-based nanomaterials such as carbon nanotubes have attracted great attention as substrates for decorating with functional groups or doping with heteroatoms. In this paper, oxidized multi-walled carbon nanotubes were modified with nitrogen at 900 degrees C and applied in direct dehydrogenation of isobutane. Upon surface oxidization and high temperature annealing, the 1.93 atom% nitrogen-doped oxidized multiwalled carbon nanotubes are found to be an effective dehydrogenation catalyst, which exhibits an isobutane conversion of 51.8% (17.4 mmol g(-1) h(-1)), isobutene selectivity and yield of 45.9% and 23.8% (8.0 mmol g(-1) h(-1)) respectively. The increased catalytic performance is well-correlated with enhanced adsorption strength of isobutane and reduced adsorption strength of isobutene, which relates to the presence of nitrogen species, as revealed by XPS and TPD measurements. Minimal deactivation of the catalyst, as indicated by time on stream studies, may be caused by the loss of nitrogen heteroatoms and the change in I-D/I-G.
引用
收藏
页码:8562 / 8570
页数:9
相关论文
共 49 条
[31]   BASIC SURFACE OXIDES ON CARBON .2. STOICHIOMETRY AND REACTION KINETICS OF FORMATION - THERMAL DEGRADATION [J].
VOLL, M ;
BOEHM, HP .
CARBON, 1970, 8 (06) :741-&
[32]   A three-dimensional porous LiFePO4 cathode material modified with a nitrogen-doped graphene aerogel for high-power lithium ion batteries [J].
Wang, Bo ;
Al Abdulla, Wael ;
Wang, Dianlong ;
Zhao, X. S. .
ENERGY & ENVIRONMENTAL SCIENCE, 2015, 8 (03) :869-875
[33]   Highly Efficient Metal Sulfide Catalysts for Selective Dehydrogenation of Isobutane to Isobutene [J].
Wang, Guowei ;
Li, Chunyi ;
Shan, Honghong .
ACS CATALYSIS, 2014, 4 (04) :1139-1143
[34]   Multi-Walled Carbon Nanotubes as a Catalyst for Gas-Phase Oxidation of Ethanol to Acetaldehyde [J].
Wang, Jia ;
Huang, Rui ;
Feng, Zhenbao ;
Liu, Hongyang ;
Su, Dangsheng .
CHEMSUSCHEM, 2016, 9 (14) :1820-1826
[35]   Hybrid Nanocarbon as a Catalyst for Direct Dehydrogenation of Propane: Formation of an Active and Selective Core-Shell sp2/sp3 Nanocomposite Structure [J].
Wang, Rui ;
Sun, Xiaoyan ;
Zhang, Bingsen ;
Sun, Xiaoying ;
Su, Dangsheng .
CHEMISTRY-A EUROPEAN JOURNAL, 2014, 20 (21) :6324-6331
[36]   Template-free synthesis of hollow nitrogen-doped carbon as efficient electrocatalysts for oxygen reduction reaction [J].
Wu, Rui ;
Chen, Siguo ;
Zhang, Yuanliang ;
Wang, Yao ;
Ding, Wei ;
Li, Li ;
Qi, Xueqiang ;
Shen, Xiu ;
Wei, Zidong .
JOURNAL OF POWER SOURCES, 2015, 274 :645-650
[37]   Investigation of the selective sites on graphitic carbons for oxidative dehydrogenation of isobutane [J].
Xie, Hong ;
Wu, Zili ;
Overbury, Steven H. ;
Liang, Chengdu ;
Schwartz, Viviane .
JOURNAL OF CATALYSIS, 2009, 267 (02) :158-166
[38]   Catalytic dehydrogenation of isobutane in the presence of hydrogen over Cs-modified Ni2P supported on active carbon [J].
Xu, Yanli ;
Sang, Huanxin ;
Wang, Kang ;
Wang, Xitao .
APPLIED SURFACE SCIENCE, 2014, 316 :163-170
[39]   N-doped carbon layer coated thermally exfoliated graphene and its capacitive behavior in redox active electrolyte [J].
Yan, Yinan ;
Kuila, Tapas ;
Kim, Nam Hoon ;
Lee, Seung Hee ;
Lee, Joong Hee .
CARBON, 2015, 85 :60-71
[40]   Raman spectra of MWCNTs and MWCNT-based H2-adsorbing system [J].
Zhang, HB ;
Lin, GD ;
Zhou, ZH ;
Dong, X ;
Chen, T .
CARBON, 2002, 40 (13) :2429-2436