Efficiency and reactivity pattern of ceria-based noble metal and transition metal-oxide catalysts in the wet air oxidation of phenol

被引：43
作者：
Arena, Francesco [1 ,2 ]
Italiano, Cristina [1 ]
Spadaro, Lorenzo [1 ,2 ]
机构：
[1] Univ Messina, Dipartimento Chim Ind & Ingn Mat, I-98166 Messina, Italy
[2] Ist CNR ITAE Nicola Giordano, I-98126 St Lucia, Italy
来源：
APPLIED CATALYSIS B-ENVIRONMENTAL | 2012年 / 115卷
关键词：
Catalytic wet air oxidation (CWAO); Phenol; Transition-metal oxide catalysts; Noble-metal catalysts; Activity; Selectivity; Stability; Reaction mechanism; Kinetics; RAY PHOTOELECTRON-SPECTROSCOPY; CARBONACEOUS DEPOSITS; REACTOR DESIGN; OXYGEN CWAO; MN; MANGANESE; DEACTIVATION; TECHNOLOGIES; MECHANISM; REMOVAL;
D O I：
10.1016/j.apcatb.2011.12.035
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：
The activity-stability pattern of ceria-based noble metal (Pt/CeO2) and transition metal-oxide (MnCeOx) catalysts in the wet air oxidation of phenol (CWAO) at different catalyst-to-phenol weight ratio (R, 1-5) was comparatively probed using a stirred batch reactor with continuous oxygen feed (T-R, 150 degrees C; Po-2. 0.9 MPa). Both Pt/CeO2 and MnCeOx systems drive a surface dual-site Langmuir-Hinshelwood (L-H) reaction path enabling higher efficiency, different reaction kinetics and "phenol-total organic carbon" conversion relationships in comparison to homogeneous CWAO catalysts [1]. A simplified reaction scheme based on consecutive adsorption and mineralization steps and the relative kinetic analysis show that the former determines the rate of phenol and TOC removal, while the latter controls the selectivity and rate of catalyst fouling. The MnCeOx system ensures a fast and complete phenol conversion and a TOC removal higher than 80% at any R, while improved adsorption and mineralization functionalities explain a higher resistance to deactivation by fouling than Pt/CeO2 system. (C) 2011 Elsevier B.V. All rights reserved.
引用
收藏
页码：336 / 345
页数：10
相关论文
共 38 条
[1]   Cerium incorporated ordered manganese oxide OMS-2 materials: Improved catalysts for wet oxidation of phenol compounds [J].
Abecassis-Wolfovich, M ;
Jothiramalingam, R ;
Landau, MV ;
Herskowitz, M ;
Viswanathan, B ;
Varadarajan, TK .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2005, 59 (1-2) :91-98
[2]   Catalytic wet oxidation of phenol with Mn-Ce-based oxide catalysts: Impact of reactive adsorption on TOC removal [J].
Abecassis-Wolfovich, M ;
Landau, MV ;
Brenner, A ;
Herskowitz, M .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2004, 43 (17) :5089-5097
[3]   Basic evaluation of the catalytic pattern of the CuCeOx system in the wet oxidation of phenol with oxygen [J].
Arena, F ;
Alongi, E ;
Famulari, P ;
Parmaliana, A ;
Trunfio, G .
CATALYSIS LETTERS, 2006, 107 (1-2) :39-46
[4]   Activity and resistance to leaching of Cu-based catalysts in the wet oxidation of phenol [J].
Arena, F ;
Giovenco, R ;
Torre, T ;
Venuto, A ;
Parmaliana, A .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2003, 45 (01) :51-62
[5]  
Arena F., 2006, STUD SURF SCI CATAL, V172, P489
[6]  
Arena F., 2010, ENV ENG SUSTAINABILI, P297
[7]   Improved MnCeOx systems for the catalytic wet oxidation (CWO) of phenol in wastewater streams [J].
Arena, Francesco ;
Negro, Jacopo ;
Parmaliana, Adolfo ;
Spadaro, Lorenzo ;
Trunfio, Giuseppe .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2007, 46 (21) :6724-6731
[8]   Mechanistic and kinetic insights into the wet air oxidation of phenol with oxygen (CWAO) by homogeneous and heterogeneous transition-metal catalysts [J].
Arena, Francesco ;
Italian, Cristina ;
Raneri, Antonino ;
Saja, Concetta .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2010, 99 (1-2) :321-328
[9]   Nanosize Effects, Physicochemical Properties, And Catalytic Oxidation Pattern of the Redox-Precipitated MnCeOx System [J].
Arena, Francesco ;
Trunfio, Giuseppe ;
Fazio, Barbara ;
Negro, Jacopo ;
Spadaro, Lorenzo .
JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (07) :2822-2829
[10]   Optimization of the MnCeOx system for the catalytic wet oxidation of phenol with oxygen (CWAO) [J].
Arena, Francesco ;
Trunfio, Giuseppe ;
Negro, Jacopo ;
Spadaro, Lorenzo .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2008, 85 (1-2) :40-47
1234