Catalytic properties of CuMgAlO catalyst and degradation mechanism in CWPO of methyl orange

被引:74
作者
Han, Jing [1 ]
Zeng, Hong-Yan [1 ]
Xu, Sheng [1 ]
Chen, Chao-Rong [1 ]
Liu, Xiao-Jun [1 ]
机构
[1] Xiangtan Univ, Coll Chem Engn, Xiangtan 411105, Hunan, Peoples R China
关键词
CWPO; Degeneration process; CuMgAlO catalyst; Methyl orange; WET PEROXIDE OXIDATION; MG-AL HYDROTALCITE; INDUCED PHOTOCATALYTIC ACTIVITY; AZO DYES; MIXED OXIDES; ENVIRONMENTAL REMEDIATION; BASE CATALYSTS; AIR OXIDATION; PHENOL; CU;
D O I
10.1016/j.apcata.2016.08.015
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
Cu-loaded MgAl hydrotalcite catalysts were synthesized by impregnation method and further used for catalytic wet peroxidation (CWPO) of methyl orange (MO) using hydrogen peroxide as oxidant. The synthesized catalysts have been characterized by XRD, SEM/EDS, TG/DTA, XPS, H-2-TPR and BET. The characterizations showed that a good dispersion of Cu species inside the MgAl hydrotalcite supports, where Cu2+ and Cu+ species were coexistence, mainly existed as Cu2+ <-> Cu+ pairs. The CuMgAlO catalyst showed the highest catalytic activity due to the high content of Cu2+ <-> Cu+ pairs, stable performance during reuse for five cycles with fewer copper leaching. The degradation mechanism of MO was determined by UV-vis, ATR-FTIR and GC-MS. The hydroxyl radicals (HO center dot) induced strong oxidizing effect, where the azo groups (-N=N-) double bonds would be first attacked by the hydroxyl radical and other free radicals. With the continuous oxidization, these intermediates could be oxidized to the final oxidation products, such as water and carbon dioxide. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:72 / 80
页数:9
相关论文
共 50 条
[1]   Low-temperature combustion of 2,4,6-trichlorophenol in catalytic wet oxidation with nanocasted Mn-Ce-oxide catalyst [J].
Abecassis-Wolfovich, M. ;
Landau, M. V. ;
Brenner, A. ;
Herskowitz, M. .
JOURNAL OF CATALYSIS, 2007, 247 (02) :201-213
[2]   Reduction of NOx in C3H6/air mixtures over Cu/Al2O3 catalysts [J].
Anderson, JA ;
Marquez-Alvarez, C ;
Lopez-Munoz, MJ ;
Rodriguez-Ramos, I ;
Guerrero-Ruiz, A .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 14 (3-4) :189-202
[3]   Influence of co-bivalent ions in Cu-containing LDHs and solvent on hydroxylation of benzene to phenol [J].
Antonyraj, Churchil A. ;
Kannan, S. .
APPLIED CLAY SCIENCE, 2011, 53 (02) :297-304
[4]   Phenol Hydroxylation over Cu-Containing LDHs and Their Calcined Forms: Profound Cobivalent Metal Influence [J].
Antonyraj, Churchil A. ;
Gandhi, Mohini ;
Kannan, S. .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2010, 49 (13) :6020-6026
[5]   Heterogeneous coupling of phenylethyne over Cu-Mg-Al mixed oxides - Influence of catalyst composition and calcination temperature on structural and catalytic properties [J].
Auer, SM ;
Wandeler, R ;
Gobel, U ;
Baiker, A .
JOURNAL OF CATALYSIS, 1997, 169 (01) :1-12
[6]   Catalytic wet peroxide oxidation (CWPO) of phenol over mixed (Al-Cu)-pillared clays [J].
Barrault, J ;
Bouchoule, C ;
Echachoui, K ;
Frini-Srasra, N ;
Trabelsi, M ;
Bergaya, F .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1998, 15 (3-4) :269-274
[7]   Catalytic wet peroxide oxidation over mixed (Al-Fe) pillared clays [J].
Barrault, J ;
Abdellaoui, M ;
Bouchoule, C ;
Majesté, A ;
Tatibouët, JM ;
Louloudi, A ;
Papayannakos, N ;
Gangas, NH .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2000, 27 (04) :L225-L230
[8]   Cu Mixed Oxides Based on Hydrotalcite-Like Compounds for the Oxidation of Trichloroethylene [J].
Blanch-Raga, Neus ;
Eduardo Palomares, A. ;
Martinez-Triguero, Joaquin ;
Fetter, Geolar ;
Bosch, Pedro .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2013, 52 (45) :15772-15779
[9]   Catalytic wet peroxide oxidation of phenol over Al-Cu or Al-Fe modified clays [J].
Carriazo, JG ;
Guelou, E ;
Barrault, J ;
Tatibouët, JM ;
Moreno, S .
APPLIED CLAY SCIENCE, 2003, 22 (06) :303-308
[10]   HYDROTALCITE-TYPE ANIONIC CLAYS: PREPARATION, PROPERTIES AND APPLICATIONS [J].
Cavani, F. ;
Trifiro, F. ;
Vaccari, A. .
CATALYSIS TODAY, 1991, 11 (02) :173-301