Green Chemistry for the Transformation of Chlorinated Wastes: Catalytic Hydrodechlorination on Pd-Ni and Pd-Fe Bimetallic Catalysts Supported on SiO<sub>2</sub>

Monometallic catalysts based on Fe, Ni and Pd, as well as bimetallic catalysts based on Fe-Pd and based on Ni-Pd supported on silica, were synthesized using a sol–gel cogelation process. These catalysts were tested in chlorobenzene hydrodechlorination at low conversion to consider a differential rea...

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Main Authors: Julien G. Mahy, Thierry Delbeuck, Kim Yên Tran, Benoît Heinrichs, Stéphanie D. Lambert
Format: Article
Language:English
Published: MDPI AG 2023-03-01
Series:Gels
Subjects:
Online Access:https://www.mdpi.com/2310-2861/9/4/275
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author Julien G. Mahy
Thierry Delbeuck
Kim Yên Tran
Benoît Heinrichs
Stéphanie D. Lambert
author_facet Julien G. Mahy
Thierry Delbeuck
Kim Yên Tran
Benoît Heinrichs
Stéphanie D. Lambert
author_sort Julien G. Mahy
collection DOAJ
description Monometallic catalysts based on Fe, Ni and Pd, as well as bimetallic catalysts based on Fe-Pd and based on Ni-Pd supported on silica, were synthesized using a sol–gel cogelation process. These catalysts were tested in chlorobenzene hydrodechlorination at low conversion to consider a differential reactor. In all samples, the cogelation method allowed very small metallic nanoparticles of 2–3 nm to be dispersed inside the silica matrix. Nevertheless, the presence of some large particles of pure Pd was noted. The catalysts had specific surface areas between 100 and 400 m<sup>2</sup>/g. In view of the catalytic results obtained, the Pd-Ni catalysts are less active than the monometallic Pd catalyst (<6% of conversion) except for catalysts with a low proportion of Ni (9% of conversion) and for reaction temperatures above 240 °C. In this series of catalysts, increasing the Ni content increases the activity but leads to an amplification of the catalyst deactivation phenomenon compared to Pd alone. On the other hand, Pd-Fe catalysts are more active with a double conversion value compared to a Pd monometallic catalyst (13% vs. 6%). The difference in the results obtained for each of the catalysts in the Pd-Fe series could be explained by the greater presence of the Fe-Pd alloy in the catalyst. Fe would have a cooperative effect when associated with Pd. Although Fe is inactive alone for chlorobenzene hydrodechlorination, when Fe is coupled to another metal from the group VIIIb, such as Pd, it allows the phenomenon of Pd poisoning by HCl to be reduced.
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spelling doaj.art-b5ed09542aae46c3ab1ff3b954ff889b2023-11-17T19:21:09ZengMDPI AGGels2310-28612023-03-019427510.3390/gels9040275Green Chemistry for the Transformation of Chlorinated Wastes: Catalytic Hydrodechlorination on Pd-Ni and Pd-Fe Bimetallic Catalysts Supported on SiO<sub>2</sub>Julien G. Mahy0Thierry Delbeuck1Kim Yên Tran2Benoît Heinrichs3Stéphanie D. Lambert4Department of Chemical Engineering—Nanomaterials, Catalysis & Electrochemistry, University of Liège, B6a, Quartier Agora, Allée du six Août 11, 4000 Liège, BelgiumDepartment of Chemical Engineering—Nanomaterials, Catalysis & Electrochemistry, University of Liège, B6a, Quartier Agora, Allée du six Août 11, 4000 Liège, BelgiumDepartment of Chemical Engineering—Nanomaterials, Catalysis & Electrochemistry, University of Liège, B6a, Quartier Agora, Allée du six Août 11, 4000 Liège, BelgiumDepartment of Chemical Engineering—Nanomaterials, Catalysis & Electrochemistry, University of Liège, B6a, Quartier Agora, Allée du six Août 11, 4000 Liège, BelgiumDepartment of Chemical Engineering—Nanomaterials, Catalysis & Electrochemistry, University of Liège, B6a, Quartier Agora, Allée du six Août 11, 4000 Liège, BelgiumMonometallic catalysts based on Fe, Ni and Pd, as well as bimetallic catalysts based on Fe-Pd and based on Ni-Pd supported on silica, were synthesized using a sol–gel cogelation process. These catalysts were tested in chlorobenzene hydrodechlorination at low conversion to consider a differential reactor. In all samples, the cogelation method allowed very small metallic nanoparticles of 2–3 nm to be dispersed inside the silica matrix. Nevertheless, the presence of some large particles of pure Pd was noted. The catalysts had specific surface areas between 100 and 400 m<sup>2</sup>/g. In view of the catalytic results obtained, the Pd-Ni catalysts are less active than the monometallic Pd catalyst (<6% of conversion) except for catalysts with a low proportion of Ni (9% of conversion) and for reaction temperatures above 240 °C. In this series of catalysts, increasing the Ni content increases the activity but leads to an amplification of the catalyst deactivation phenomenon compared to Pd alone. On the other hand, Pd-Fe catalysts are more active with a double conversion value compared to a Pd monometallic catalyst (13% vs. 6%). The difference in the results obtained for each of the catalysts in the Pd-Fe series could be explained by the greater presence of the Fe-Pd alloy in the catalyst. Fe would have a cooperative effect when associated with Pd. Although Fe is inactive alone for chlorobenzene hydrodechlorination, when Fe is coupled to another metal from the group VIIIb, such as Pd, it allows the phenomenon of Pd poisoning by HCl to be reduced.https://www.mdpi.com/2310-2861/9/4/275noble metalenvironmental catalysissol–gel processporous materialsgreen chemistry
spellingShingle Julien G. Mahy
Thierry Delbeuck
Kim Yên Tran
Benoît Heinrichs
Stéphanie D. Lambert
Green Chemistry for the Transformation of Chlorinated Wastes: Catalytic Hydrodechlorination on Pd-Ni and Pd-Fe Bimetallic Catalysts Supported on SiO<sub>2</sub>
Gels
noble metal
environmental catalysis
sol–gel process
porous materials
green chemistry
title Green Chemistry for the Transformation of Chlorinated Wastes: Catalytic Hydrodechlorination on Pd-Ni and Pd-Fe Bimetallic Catalysts Supported on SiO<sub>2</sub>
title_full Green Chemistry for the Transformation of Chlorinated Wastes: Catalytic Hydrodechlorination on Pd-Ni and Pd-Fe Bimetallic Catalysts Supported on SiO<sub>2</sub>
title_fullStr Green Chemistry for the Transformation of Chlorinated Wastes: Catalytic Hydrodechlorination on Pd-Ni and Pd-Fe Bimetallic Catalysts Supported on SiO<sub>2</sub>
title_full_unstemmed Green Chemistry for the Transformation of Chlorinated Wastes: Catalytic Hydrodechlorination on Pd-Ni and Pd-Fe Bimetallic Catalysts Supported on SiO<sub>2</sub>
title_short Green Chemistry for the Transformation of Chlorinated Wastes: Catalytic Hydrodechlorination on Pd-Ni and Pd-Fe Bimetallic Catalysts Supported on SiO<sub>2</sub>
title_sort green chemistry for the transformation of chlorinated wastes catalytic hydrodechlorination on pd ni and pd fe bimetallic catalysts supported on sio sub 2 sub
topic noble metal
environmental catalysis
sol–gel process
porous materials
green chemistry
url https://www.mdpi.com/2310-2861/9/4/275
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