Highly dispersed Fe3+-Al2O3 for the Fenton-like oxidation of phenol in a continuous up-flow fixed bed reactor: enhancing catalyst stability through operating conditions

A highly dispersed Fe3+-Al2O3 catalyst (6 wt% Fe) was used for the catalytic wet hydrogen peroxide oxidation of phenol (1 g/L) in an up-flow fixed bed reactor (UFBR) under continuous operation. To enhance catalytic performance, three simple synthesis strategies were combined: two-stage impregnation...

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Detalles Bibliográficos
Autores principales: Di Luca, Carla, Massa, Paola Andrea, Grau, Javier Mario, Marchetti, Sergio Gustavo, Fenoglio, Rosa Juana, Haure, Patricia Mónica
Formato: Articulo
Lenguaje:Inglés
Publicado: 2018
Materias:
Química
Catalyst deactivation
Chelating intermediates
Continuous fixed bed reactor
Fe3+-al2o3
Phenol removal
Acceso en línea:http://sedici.unlp.edu.ar/handle/10915/102643
https://ri.conicet.gov.ar/11336/84117
Aporte de:
SEDICI (UNLP) de Universidad Nacional de La Plata
id I19-R120-10915-102643
record_format dspace
institution Universidad Nacional de La Plata
institution_str I-19
repository_str R-120
collection SEDICI (UNLP)
language Inglés
topic Química
Catalyst deactivation
Chelating intermediates
Continuous fixed bed reactor
Fe3+-al2o3
Phenol removal
spellingShingle Química
Catalyst deactivation
Chelating intermediates
Continuous fixed bed reactor
Fe3+-al2o3
Phenol removal
Di Luca, Carla
Massa, Paola Andrea
Grau, Javier Mario
Marchetti, Sergio Gustavo
Fenoglio, Rosa Juana
Haure, Patricia Mónica
Highly dispersed Fe3+-Al2O3 for the Fenton-like oxidation of phenol in a continuous up-flow fixed bed reactor: enhancing catalyst stability through operating conditions
topic_facet Química
Catalyst deactivation
Chelating intermediates
Continuous fixed bed reactor
Fe3+-al2o3
Phenol removal
description A highly dispersed Fe3+-Al2O3 catalyst (6 wt% Fe) was used for the catalytic wet hydrogen peroxide oxidation of phenol (1 g/L) in an up-flow fixed bed reactor (UFBR) under continuous operation. To enhance catalytic performance, three simple synthesis strategies were combined: two-stage impregnation of iron citrate, acid washing with CH3COOH and thermal treatment at 900 °C. Solid samples were characterized in depth by several techniques: N2 Physisorption, XRD, SEM–EDAX, TEM, TGA, PZC, TPD of pyridine, XPS and Mössbauer. Peroxidation experiments were performed in an UFBR over a wide range of operating parameters in order to evaluate their influence on phenol mineralization and catalyst stability. Under selected operating condition (T = 90 °C, Wcat = 20 g, QL = 1.2 mL/min and [H2O2]:[Phenol] = 16.8), complete phenol conversion and remarkable TOC reduction of 90% were achieved, with a high H2O2 consumption efficiency (η = 76%) and low Fe leaching (< 3 mg/L). After 70 h of usage at different steady state conditions, the catalyst retained high mineralization levels (XTOC> 70%) but the cumulative iron loss was calculated to be c.a. 20% of the initial Fe loaded in the UFBR. The catalyst was susceptible to leaching due to the accumulation of complexing intermediates such as carboxylic acids. However, acceptable iron leaching values (< 10 mg/L) were achieved when the reactor operating conditions were properly set (55% < XTOC> 80%). The presence of chelating by-products favored also the Fe redistribution inside the catalyst pellets. Nevertheless, catalyst decay in the long-term operation was mainly due to the occurrence and permanence of chelating organic acids. This process was specially promoted by the amphoteric character of the alumina-based catalyst. However, adsorbed species were promptly eliminated by calcination at 500 °C, recovering steady state conversion profiles.
format Articulo
Articulo
author Di Luca, Carla
Massa, Paola Andrea
Grau, Javier Mario
Marchetti, Sergio Gustavo
Fenoglio, Rosa Juana
Haure, Patricia Mónica
author_facet Di Luca, Carla
Massa, Paola Andrea
Grau, Javier Mario
Marchetti, Sergio Gustavo
Fenoglio, Rosa Juana
Haure, Patricia Mónica
author_sort Di Luca, Carla
title Highly dispersed Fe3+-Al2O3 for the Fenton-like oxidation of phenol in a continuous up-flow fixed bed reactor: enhancing catalyst stability through operating conditions
title_short Highly dispersed Fe3+-Al2O3 for the Fenton-like oxidation of phenol in a continuous up-flow fixed bed reactor: enhancing catalyst stability through operating conditions
title_full Highly dispersed Fe3+-Al2O3 for the Fenton-like oxidation of phenol in a continuous up-flow fixed bed reactor: enhancing catalyst stability through operating conditions
title_fullStr Highly dispersed Fe3+-Al2O3 for the Fenton-like oxidation of phenol in a continuous up-flow fixed bed reactor: enhancing catalyst stability through operating conditions
title_full_unstemmed Highly dispersed Fe3+-Al2O3 for the Fenton-like oxidation of phenol in a continuous up-flow fixed bed reactor: enhancing catalyst stability through operating conditions
title_sort highly dispersed fe3+-al2o3 for the fenton-like oxidation of phenol in a continuous up-flow fixed bed reactor: enhancing catalyst stability through operating conditions
publishDate 2018
url http://sedici.unlp.edu.ar/handle/10915/102643
https://ri.conicet.gov.ar/11336/84117
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