Metal-doped carbon aerogels as catalysts during ozonation processes in aqueous solutions

被引:60
作者
Sanchez-Polo, M.
Rivera-Utrilla, J.
von Gunten, U.
机构
[1] Swiss Fed Inst Aquat Sci & Technol, EAWAG, CH-8600 Dubendorf, Switzerland
[2] Univ Granada, Dept Quim Inorgan, F Ciencias, E-18071 Granada, Spain
关键词
ozonation; carbon aerogels; transition metals; p-chlorobenzoate (pCBA); (OH)-O-center dot radicals;
D O I
10.1016/j.watres.2006.07.020
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The efficiency of Co(II)-, Mn(II)-, and Ti(IV)-doped carbon aerogels for the transformation of ozone into center dot OH radicals was investigated. The carbon aerogels had a markedly acid surface character (pH(PZC)congruent to 3-4) with very high surface oxygen concentrations (O congruent to 20%). X-ray photoelectron spectroscopy (XPS) analyses of the samples showed the oxidation state of the metals was +2 for Co and Mn and +4 for Ti. The presence of Mn(II)-doped carbon aerogel enhanced ozone transformation into (OH)-O-center dot radicals, whereas the presence of Co(II) and 71(IV) carbon aerogels presented no activity in this process. Moreover, it was observed that an increase in the concentration of Mn in the surface of the aerogel increases its efficiency to transform ozone into (OH)-O-center dot radicals, with an Rct value ([OH]/[O-3]) of 5.36 x 10(-8) for the aerogel doped with 16% of surface Mn(II) compared to an R-ct of 2.68 x 10(-9) for conventional ozonation. Regardless of the aerogel used, XPS analysis of the ozonated aerogel samples showed an increase in the concentration of surface oxygen when the exposure to ozone was longer. However, presence of oxidized metal species after ozone treatment was only detected in the case of the Mn-doped aerogel, (Mn(III) and Mn(IV)). CO2 activation of carbon aerogel produced a marked increase in its efficiency to transform ozone into (OH)-O-center dot radicals compared with non-activated sample. The efficiency of Mn activated carbon aerogel to transform ozone into (OH)-O-center dot radicals was greater than that of Witco commercial activated carbon or H2O2 in the ozonation of water from Lake Zurich (Zurich, Switzerland). (c) 2006 Elsevier Ltd. All rights reserved.
引用
收藏
页码:3375 / 3384
页数:10
相关论文
共 39 条
[1]   DECOLORIZATION BY OZONE OF DIRECT DYES IN PRESENCE OF SOME CATALYSTS [J].
ABDO, MSE ;
SHABAN, H ;
BADER, MSH .
JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH PART A-ENVIRONMENTAL SCIENCE AND ENGINEERING & TOXIC AND HAZARDOUS SUBSTANCE CONTROL, 1988, 23 (07) :697-710
[2]   THE KINETICS OF MN(II)-CATALYZED OZONATION OF OXALIC-ACID IN AQUEOUS-SOLUTION [J].
ANDREOZZI, R ;
INSOLA, A ;
CAPRIO, V ;
DAMORE, MG .
WATER RESEARCH, 1992, 26 (07) :917-921
[3]   The use of manganese dioxide as a heterogeneous catalyst for oxalic acid ozonation in aqueous solution [J].
Andreozzi, R ;
Insola, A ;
Caprio, V ;
Marotta, R ;
Tufano, V .
APPLIED CATALYSIS A-GENERAL, 1996, 138 (01) :75-81
[4]   DETERMINATION OF OZONE IN WATER BY THE INDIGO METHOD - A SUBMITTED STANDARD METHOD [J].
BADER, H ;
HOIGNE, J .
OZONE-SCIENCE & ENGINEERING, 1982, 4 (04) :169-176
[5]   A TiO2/Al2O3 catalyst to improve the ozonation of oxalic acid in water [J].
Beltrán, FJ ;
Rivas, FJ ;
Montero-de-Espinosa, R .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2004, 47 (02) :101-109
[6]   Kinetics of heterogeneous catalytic ozone decomposition in water on an activated carbon [J].
Beltrán, FJ ;
Rivas, J ;
Alvarez, P ;
Montero-de-Espinosa, R .
OZONE-SCIENCE & ENGINEERING, 2002, 24 (04) :227-237
[7]  
BRUNUY R, 1994, OZONE-SCI ENG, V6, P163
[8]   Catalytic oxidation of benzene with ozone over alumina-supported manganese oxides [J].
Einaga, H ;
Futamura, S .
JOURNAL OF CATALYSIS, 2004, 227 (02) :304-312
[9]   Hydroxyl radical ozone ratios during ozonation processes.: I-The Rct concept [J].
Elovitz, MS ;
von Gunten, U .
OZONE-SCIENCE & ENGINEERING, 1999, 21 (03) :239-260
[10]   XPS study of copper-doped carbon aerogels [J].
Fu, RW ;
Yoshizawa, N ;
Dresselhaus, MS ;
Dresselhaus, G ;
Satcher, JH ;
Baumann, TF .
LANGMUIR, 2002, 18 (26) :10100-10104