Active Coordinatively Unsaturated Manganese Monoxide-Containing Mesoporous Carbon Catalyst in Wet Peroxide Oxidation

被引:55
作者
Kong, Lina [1 ,2 ]
Wei, Wei [1 ,2 ]
Zhao, Qingfei [1 ,2 ]
Wang, Jian-Qiang [3 ]
Wan, Ying [1 ,2 ]
机构
[1] Shanghai Normal Univ, Shanghai Key Lab Rare Earth Funct Mat, Minist Educ, Key Lab Resource Chem, Shanghai 200234, Peoples R China
[2] Shanghai Normal Univ, Dept Chem, Shanghai 200234, Peoples R China
[3] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
来源
ACS CATALYSIS | 2012年 / 2卷 / 12期
基金
美国国家科学基金会;
关键词
manganese monoxide; carbon; mesostructure; coordinative unsaturation; confinement; oxidation; SIZE-SELECTIVE SYNTHESIS; HETEROGENEOUS CATALYSIS; HYDROGEN-PEROXIDE; PHENOL; SILICA; NANOPARTICLES; IRON; CRYSTALLINE; COMPOSITES; MESOPHASES;
D O I
10.1021/cs300534y
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
A novel heterogeneous coordinatively unsaturated manganese monoxide-containing mesoporous carbon catalyst (C-MnO) is reported here. The catalysts exhibit high catalytic activity in wet oxidation of phenol (almost complete mineralization with an initial concentration of 50 mg/L at atmospheric pressure) and stability (reused 20 times without obvious activity loss or metal leaching), and they take more advantages than most developed heterogeneous Fenton catalysts. The one-pot surfactant self-assembly approach is used for the synthesis of the mesoporous C-MnO catalysts. Small-angle X-ray diffraction (XRD), N-2 sorption, and transmission electron microscopy results reveal that the catalysts have the ordered two-dimensional hexagonal mesostructure, large surface areas (530-552 m(2)/g), uniform pore sizes (3.3-5.4 nm), and large pore volumes (0.34-0.44 cm(3)/g); MnO nanoparticles (<12 nm) are well dispersed inside carbon mesopore systems with high crystallinity. The wide-angle XRD pattern reveals the presence of cubic rock salt structure MnO, and the Mn K-edge X-ray absorption fine structure spectra confirms the low chemical valence and the coordination unsaturated state of Mn. The high activity and stability of C-MnO catalysts might be related to the mesostructure, carbon pore wall, and, more importantly, the confined undercoordinative MnO nanoparticles.
引用
收藏
页码:2577 / 2586
页数:10
相关论文
共 63 条
[31]   Heterogeneous catalytic wet peroxide oxidation systems for the treatment of an industrial pharmaceutical wastewater [J].
Melero, J. A. ;
Martinez, F. ;
Botas, J. A. ;
Molina, R. ;
Pariente, M. I. .
WATER RESEARCH, 2009, 43 (16) :4010-4018
[32]   Ordered mesoporous polymers and homologous carbon frameworks: Amphiphilic surfactant templating and direct transformation [J].
Meng, Y ;
Gu, D ;
Zhang, FQ ;
Shi, YF ;
Yang, HF ;
Li, Z ;
Yu, CZ ;
Tu, B ;
Zhao, DY .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2005, 44 (43) :7053-7059
[33]  
Meng Y., 2005, ANGEW CHEM, V117, P7215, DOI DOI 10.1002/ANGE.200501561
[34]   A family of highly ordered mesoporous polymer resin and carbon structures from organic-organic self-assembly [J].
Meng, Yan ;
Gu, Dong ;
Zhang, Fuqiang ;
Shi, Yifeng ;
Cheng, Liang ;
Feng, Dan ;
Wu, Zhangxiong ;
Chen, Zhenxia ;
Wan, Ying ;
Stein, Andreas ;
Zhao, Dongyuan .
CHEMISTRY OF MATERIALS, 2006, 18 (18) :4447-4464
[35]   Enhancement of the Catalytic Activity of Supported Gold Nanoparticles for the Fenton Reaction by Light [J].
Navalon, Sergio ;
de Miguel, Maykel ;
Martin, Roberto ;
Alvaro, Mercedes ;
Garcia, Hermenegildo .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2011, 133 (07) :2218-2226
[36]   Heterogeneous Fenton catalysts based on clays, silicas and zeolites [J].
Navalon, Sergio ;
Alvaro, Mercedes ;
Garcia, Hermenegildo .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2010, 99 (1-2) :1-26
[37]   Wet peroxide oxidation of phenolic solutions over different iron-containing zeolitic materials [J].
Ovejero, G ;
Sotelo, JL ;
Martínez, F ;
Melero, JA ;
Gordo, L .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2001, 40 (18) :3921-3928
[38]   On the True Photoreactivity Order of {001}, {010}, and {101} Facets of Anatase TiO2 Crystals [J].
Pan, Jian ;
Liu, Gang ;
Lu, Gao Qing ;
Cheng, Hui-Ming .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (09) :2133-2137
[39]  
Plant L., 1994, CHEM ENG, V101, P16
[40]  
Quintanilla A., 2012, APPL CATAL B-ENVIRON, V111-112, P81