Covalent triazine-based framework as an efficient catalyst support for ammonia decomposition

被引:30
作者
Chang, Fei [1 ,2 ]
Guo, Jianping [1 ,2 ]
Wu, Guotao [1 ]
Liu, Lin [1 ]
Zhang, Miao [1 ,2 ]
He, Teng [1 ]
Wang, Peikun [1 ,2 ]
Yu, Pei [1 ,2 ]
Chen, Ping [1 ,3 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
基金
中国国家自然科学基金;
关键词
RUTHENIUM CATALYSTS; CARBON NANOTUBES; STRUCTURE SENSITIVITY; OXYGEN REDUCTION; ACTIVE-CARBON; HYDROGEN; GENERATION; OXIDATION; RU; ALCOHOLS;
D O I
10.1039/c4ra12816h
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The covalent triazine-based framework (CTF), a new type of nitrogen-containing microporous polymer, was employed as a catalyst support for ammonia decomposition. Either in terms of NH3 conversion rate or turnover frequency, Ru/CTF-1 has a highly enhanced performance compared to Ru/CNTs, which rank as one of the best un-promoted catalysts reported so far. The compositional and structural information of Ru/CTF-1 and Ru/CNTs catalysts have been characterized by ICP, N-2 physisorption, XRD, TEM, XPS, and NH3-TPD techniques. Ru particles on CTF-1 and CNTs are ca. 3 nm in diameter and have a similar degree of dispersion. However, the binding energy of Ru 3p electrons is ca. 0.6 eV less for Ru/CTF-1 than that for Ru/CNTs showing significant increase in electron density in the former, which is likely due to the interaction between the nitrogen-rich groups of CTF-1 and the Ru nanoparticles. Moreover, the presence of CTF-1 enhances the chemisorption of NH3, which, together with the increased electron density of Ru, may facilitate the competitive chemisorption of NH3 and recombinative desorption of adsorbed nitrogen via lowered activation energy and thus, enable faster reaction rate.
引用
收藏
页码:3605 / 3610
页数:6
相关论文
共 37 条
[1]   SUPPORT AND PROMOTER EFFECT OF RUTHENIUM CATALYST .2. RUTHENIUM ALKALINE-EARTH CATALYST FOR ACTIVATION OF DINITROGEN [J].
AIKA, K ;
OHYA, A ;
OZAKI, A ;
INOUE, Y ;
YASUMORI, I .
JOURNAL OF CATALYSIS, 1985, 92 (02) :305-311
[2]  
Anderson J.R., 1975, Structure of metallic catalysts
[3]   Elucidation of Catalyst Support Effect for NH3 Decomposition Using Ru Nanoparticles on Nitrogen-Functionalized Carbon Nanofiber Monoliths [J].
Armenise, Sabino ;
Roldan, Laura ;
Marco, Yanila ;
Monzon, A. ;
Garcia-Bordeje, Enrique .
JOURNAL OF PHYSICAL CHEMISTRY C, 2012, 116 (50) :26385-26395
[4]   Kinetics of NH3 decomposition over well dispersed Ru [J].
Bradford, MCJ ;
Fanning, PE ;
Vannice, MA .
JOURNAL OF CATALYSIS, 1997, 172 (02) :479-484
[5]   Influence of Periodic Nitrogen Functionality on the Selective Oxidation of Alcohols [J].
Chan-Thaw, Carine E. ;
Villa, Alberto ;
Veith, Gabriel M. ;
Kailasam, Kamalakannan ;
Adamczyk, Leslie A. ;
Unocic, Raymond R. ;
Prati, Laura ;
Thomas, Arne .
CHEMISTRY-AN ASIAN JOURNAL, 2012, 7 (02) :387-393
[6]   Triazine-Based Polymers as Nanostructured Supports for the Liquid-Phase Oxidation of Alcohols [J].
Chan-Thaw, Carine E. ;
Villa, Alberto ;
Prati, Laura ;
Thomas, Arne .
CHEMISTRY-A EUROPEAN JOURNAL, 2011, 17 (03) :1052-1057
[7]   Effects of nitrogen doping on the structure of carbon nanotubes (CNTs) and activity of Ru/CNTs in ammonia decomposition [J].
Chen, Jiuling ;
Zhu, Zhong Hua ;
Wang, Shaobin ;
Ma, Qing ;
Rudolph, Victor ;
Lu, Gao Qing .
CHEMICAL ENGINEERING JOURNAL, 2010, 156 (02) :404-410
[8]   Light metals decorated covalent triazine-based frameworks as a high capacity hydrogen storage medium [J].
Chen, Xiaowei ;
Yuan, Feng ;
Gu, Qinfen ;
Yu, Xuebin .
JOURNAL OF MATERIALS CHEMISTRY A, 2013, 1 (38) :11705-11710
[9]   Identification of electron donor states in N-doped carbon nanotubes [J].
Czerw, R ;
Terrones, M ;
Charlier, JC ;
Blase, X ;
Foley, B ;
Kamalakaran, R ;
Grobert, N ;
Terrones, H ;
Tekleab, D ;
Ajayan, PM ;
Blau, W ;
Rühle, M ;
Carroll, DL .
NANO LETTERS, 2001, 1 (09) :457-460
[10]   Surface science based microkinetic analysis of ammonia synthesis over ruthenium catalysts [J].
Dahl, S ;
Sehested, J ;
Jacobsen, CJH ;
Törnqvist, E ;
Chorkendorff, I .
JOURNAL OF CATALYSIS, 2000, 192 (02) :391-399