Iron-cobalt mixed oxide nanocatalysts: Heterogeneous peroxymonosulfate activation, cobalt leaching, and ferromagnetic properties for environmental applications

被引:533
作者
Yang, Qiujing [2 ]
Choi, Hyeok [1 ]
Al-Abed, Souhail R. [1 ]
Dionysiou, Dionysios D. [2 ]
机构
[1] US EPA, Natl Risk Management Res Lab, Cincinnati, OH 45268 USA
[2] Univ Cincinnati, Dept Civil & Environm Engn, Cincinnati, OH 45221 USA
基金
美国国家科学基金会;
关键词
2,4-Dichlorophenol; Advanced oxidation processes (AOPs); Advanced oxidation technologies (AOTs); Cobalt; Fe-Co; Ferromagnetic properties; Heterogeneous reaction; Iron; Iron-cobalt; Leaching; Mixed oxide; Nanoparticles; Oxone; Peroxymonosulfate; Support materials; Sulfate radicals; Titanium dioxide; Titania; TiO2; Water treatment; Water purification; FISCHER-TROPSCH SYNTHESIS; CATALYSTS; WATER; NANOPARTICLES; DEGRADATION; PHOTOCATALYSIS; GENERATION; RADICALS; SURFACES; HYDROGEN;
D O I
10.1016/j.apcatb.2008.10.013
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
Sulfate radical-based advanced oxidation technologies (SR-AOTs) are attracting considerable attention due to the high oxidizing ability of SRs to degrade organic pollutants in aqueous environments. This study was carried out to respond to current concerns and challenges in SR-AOTs, including (i) need of heterogeneous activation of sulfate salts using transition metal oxides, (ii) nanoscaling of the metal oxide catalysts for high catalytic activity and promising properties with respect to leaching, and (iii) easy removal and recovery of the catalytic materials after their applications for water and wastewater treatments. In this study, we report a novel approach of using Fe-Co mixed oxide nanocatalysts for the heterogeneous activation of peroxymonosulfate (PMS) to generate SRs targeting the decomposition of 2,4-dichlorophenol, and especially focus on some synthesis parameters such as calcination temperature, Fe/Co contents, and TiO2 support. The physicochemical properties of the catalysts were investigated using porosimetry, XRD, HR-TEM, H-2-TPR, and XPS. Ferromagnetic CoFe2O4 composites formed by thermal oxidation of a mixed phase of Fe and Co exhibited significant implications for the efficient and environmentally friendly activation of PMS, including(i) the cobalt species in CoFe2O4 are of Co(II), unlike Co3O4 showing some detrimental effects of Co(III) on the PMS activation, (ii) CoFe2O4 possesses suppressed Co leaching properties due to strong Fe-Co interactions (i.e. Fe-Co linkages), and (iii) Fe-Co catalysts in form of CoFe2O4 are easier to recover due to the unique ferromagnetic nature of CoFe2O4. In addition, the presence of Fe was found to be beneficial for enriching hydroxyl group content on the Fe-Co catalyst surface, which is believed to facilitate the formation of Co(II)-OH complexes that are vital for heterogeneous PMS activation. (C) 2008 Elsevier B.V. All rights reserved.
引用
收藏
页码:462 / 469
页数:8
相关论文
共 33 条
[21]   Toxic potential of materials at the nanolevel [J].
Nel, A ;
Xia, T ;
Mädler, L ;
Li, N .
SCIENCE, 2006, 311 (5761) :622-627
[22]   RATE CONSTANTS FOR REACTIONS OF INORGANIC RADICALS IN AQUEOUS-SOLUTION [J].
NETA, P ;
HUIE, RE ;
ROSS, AB .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1988, 17 (03) :1027-1284
[23]   Degradation of chlorophenols by means of advanced oxidation processes:: a general review [J].
Pera-Titus, M ;
García-Molina, V ;
Baños, MA ;
Giménez, J ;
Esplugas, S .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2004, 47 (04) :219-256
[24]   Toluene ammoxidation on α-Fe2O3-based catalysts [J].
Rombi, E ;
Ferino, I ;
Monaci, R ;
Picciau, C ;
Solinas, V ;
Buzzoni, R .
APPLIED CATALYSIS A-GENERAL, 2004, 266 (01) :73-79
[25]  
Safarzadeh-Amiri A., 1996, J ADV OXID TECHNOL, V1, P18, DOI DOI 10.1515/JA0TS-1996-0105
[26]   Assessing the risks of manufactured nanomaterials [J].
Wiesner, Mark R. ;
Lowry, Greg V. ;
Alvarez, Pedro ;
Dionysiou, Dianysios ;
Biswas, Pratim .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (14) :4336-4345
[27]   New route to synthesize highly active nanocrystalline sulfated titania-silica: Synergetic effects between sulfate species and silica in enhancing the photocatalysis efficiency [J].
Xie, C ;
Yang, Q ;
Xu, Z ;
Liu, X ;
Du, Y .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (17) :8587-8592
[28]   Self-generation of tiered surfactant superstructures for one-pot synthesis of Co3O4 nanocubes and their closeand non-close-packed organizations [J].
Xu, R ;
Zeng, HC .
LANGMUIR, 2004, 20 (22) :9780-9790
[29]   Heterogeneous activation of peroxymonosulfate by supported cobalt catalysts for the degradation of 2,4-dichlorophenol in water: The effect of support, cobalt precursor, and UV radiation [J].
Yang, Qiujing ;
Choi, Hyeok ;
Chen, Yongjun ;
Dionysiou, Dionysios D. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2008, 77 (3-4) :300-307
[30]   Nanocrystalline cobalt oxide immobilized on titanium dioxide nanoparticles for the heterogeneous activation of peroxymonosulfate [J].
Yang, Qiujing ;
Choi, Hyeok ;
Dionysiou, Dionysios D. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2007, 74 (1-2) :170-178