Catalytic hydrodehalogenation of the flame retardant tetrabromobisphenol A by alumina-supported Pd, Rh and Pt catalysts

Tetrabromobisphenol A (TBBPA) is one of the most used BFRs, being characterized by a strong persistence and leading to negative effects on both the environment and human health. The aim of this work is to evaluate the feasibility of aqueous-phase catalytic hydrodehalogenation (HDH) for the fast and...

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Autores principales: Julia Nieto-Sandoval, Raquel Sanchez, Macarena Munoz, Zahara M. de Pedro, Jose A. Casas
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Publicado: Elsevier 2022
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spelling oai:doaj.org-article:2a705dec61c94c0a978e88a620e697ba2021-11-30T04:17:54ZCatalytic hydrodehalogenation of the flame retardant tetrabromobisphenol A by alumina-supported Pd, Rh and Pt catalysts2666-821110.1016/j.ceja.2021.100212https://doaj.org/article/2a705dec61c94c0a978e88a620e697ba2022-03-01T00:00:00Zhttp://www.sciencedirect.com/science/article/pii/S2666821121001277https://doaj.org/toc/2666-8211Tetrabromobisphenol A (TBBPA) is one of the most used BFRs, being characterized by a strong persistence and leading to negative effects on both the environment and human health. The aim of this work is to evaluate the feasibility of aqueous-phase catalytic hydrodehalogenation (HDH) for the fast and environmentally-friendly degradation of the brominated flame retardant TBBPA. Pd, Rh, and Pt on alumina commercial catalysts (1% wt.) were tested and reactions were performed under ambient operating conditions. TBBPA (1 mg L−1) was completely removed in short reaction times (< 5 min) using the Pd catalyst while longer reaction times were required in the case of Rh and Pt catalysts as active phase. Furthermore, although TBBPA suffered a strong adsorption on the catalyst surface, both adsorbed and free molecules reacted. Bromine balance was closed (> 95%) in 15 min using Pd/Al2O3. Nevertheless, employing Rh and Pt alumina-supported catalysts debromination of TBBPA increased progressively requiring much longer times and only 83% and 78% debromination yields were achieved after 2 h reaction, respectively. Bisphenol A (BPA), a well-known endocrine disruptor, was generated as reaction intermediate but it was further hydrogenated with both Pd and Rh catalysts, whereas it remained as reaction product with the Pt catalyst. A series reaction pathway considering both hydrodebromination and hydrogenation steps was proposed based on the obtained results. The experimental data obtained with the Pd/Al2O3 catalyst were successfully described by a pseudo-first order kinetic model, obtaining an apparent activation energy of 36 kJ mol−1. Notably, this catalyst showed a reasonable stability after three consecutive HDH runs.Julia Nieto-SandovalRaquel SanchezMacarena MunozZahara M. de PedroJose A. CasasElsevierarticleCatalytic hydrodehalogenationPd/Al2O3Pt/Al2O3Rh/Al2O3Flame retardantTeetrabromobisphenol AChemical engineeringTP155-156ENChemical Engineering Journal Advances, Vol 9, Iss , Pp 100212- (2022)
institution DOAJ
collection DOAJ
language EN
topic Catalytic hydrodehalogenation
Pd/Al2O3
Pt/Al2O3
Rh/Al2O3
Flame retardant
Teetrabromobisphenol A
Chemical engineering
TP155-156
spellingShingle Catalytic hydrodehalogenation
Pd/Al2O3
Pt/Al2O3
Rh/Al2O3
Flame retardant
Teetrabromobisphenol A
Chemical engineering
TP155-156
Julia Nieto-Sandoval
Raquel Sanchez
Macarena Munoz
Zahara M. de Pedro
Jose A. Casas
Catalytic hydrodehalogenation of the flame retardant tetrabromobisphenol A by alumina-supported Pd, Rh and Pt catalysts
description Tetrabromobisphenol A (TBBPA) is one of the most used BFRs, being characterized by a strong persistence and leading to negative effects on both the environment and human health. The aim of this work is to evaluate the feasibility of aqueous-phase catalytic hydrodehalogenation (HDH) for the fast and environmentally-friendly degradation of the brominated flame retardant TBBPA. Pd, Rh, and Pt on alumina commercial catalysts (1% wt.) were tested and reactions were performed under ambient operating conditions. TBBPA (1 mg L−1) was completely removed in short reaction times (< 5 min) using the Pd catalyst while longer reaction times were required in the case of Rh and Pt catalysts as active phase. Furthermore, although TBBPA suffered a strong adsorption on the catalyst surface, both adsorbed and free molecules reacted. Bromine balance was closed (> 95%) in 15 min using Pd/Al2O3. Nevertheless, employing Rh and Pt alumina-supported catalysts debromination of TBBPA increased progressively requiring much longer times and only 83% and 78% debromination yields were achieved after 2 h reaction, respectively. Bisphenol A (BPA), a well-known endocrine disruptor, was generated as reaction intermediate but it was further hydrogenated with both Pd and Rh catalysts, whereas it remained as reaction product with the Pt catalyst. A series reaction pathway considering both hydrodebromination and hydrogenation steps was proposed based on the obtained results. The experimental data obtained with the Pd/Al2O3 catalyst were successfully described by a pseudo-first order kinetic model, obtaining an apparent activation energy of 36 kJ mol−1. Notably, this catalyst showed a reasonable stability after three consecutive HDH runs.
format article
author Julia Nieto-Sandoval
Raquel Sanchez
Macarena Munoz
Zahara M. de Pedro
Jose A. Casas
author_facet Julia Nieto-Sandoval
Raquel Sanchez
Macarena Munoz
Zahara M. de Pedro
Jose A. Casas
author_sort Julia Nieto-Sandoval
title Catalytic hydrodehalogenation of the flame retardant tetrabromobisphenol A by alumina-supported Pd, Rh and Pt catalysts
title_short Catalytic hydrodehalogenation of the flame retardant tetrabromobisphenol A by alumina-supported Pd, Rh and Pt catalysts
title_full Catalytic hydrodehalogenation of the flame retardant tetrabromobisphenol A by alumina-supported Pd, Rh and Pt catalysts
title_fullStr Catalytic hydrodehalogenation of the flame retardant tetrabromobisphenol A by alumina-supported Pd, Rh and Pt catalysts
title_full_unstemmed Catalytic hydrodehalogenation of the flame retardant tetrabromobisphenol A by alumina-supported Pd, Rh and Pt catalysts
title_sort catalytic hydrodehalogenation of the flame retardant tetrabromobisphenol a by alumina-supported pd, rh and pt catalysts
publisher Elsevier
publishDate 2022
url https://doaj.org/article/2a705dec61c94c0a978e88a620e697ba
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