Fabrication of AuPd bimetallic nanoparticles and their effects on hydrogenation reactions

As catalytic reactions reach nearly 40 % of the world GDP, enhancing the catalytic properties of scarce metals, generating highly active, selective and durable catalysts is critical. Bimetallic AuPd NPs present enhanced activity and selectivity in hydrogenation reactions. However, the mechanisms beh...

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Main Author: B. F. Pinto, Jose Jorge
Format: Thesis (University of Nottingham only)
Language:English
Published: 2021
Subjects:
Online Access:https://eprints.nottingham.ac.uk/64771/
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author B. F. Pinto, Jose Jorge
author_facet B. F. Pinto, Jose Jorge
author_sort B. F. Pinto, Jose Jorge
building Nottingham Research Data Repository
collection Online Access
description As catalytic reactions reach nearly 40 % of the world GDP, enhancing the catalytic properties of scarce metals, generating highly active, selective and durable catalysts is critical. Bimetallic AuPd NPs present enhanced activity and selectivity in hydrogenation reactions. However, the mechanisms behind their improved catalytic properties when compare to their monometallic counterparts and the enhancement effect of Au in the alloy remains ambiguous. This thesis elucidates the synergetic effect in AuPd NPs leading to their enhanced catalytic properties towards the selective hydrogenation of CAL. The AuPd NPs were first co-deposited in IL ([C4C1Im][NTf2]) by magnetron sputtering and their structural and electronic properties characterised. Evidence of the interaction of both metals with the disruption of the Au surface plasmon resonance in the presence of Pd (UV-vis) was observed and the absence of the Au-IL interaction with the increase of Pd content (XPS). XAS experiments confirmed the presence of a core-shell structure in the AuPd NPs with the preferential interaction of the SO2 groups in the IL anion with the sputtered Pd atoms leading to an ordering of the NP structure during growth and nucleation. Highest conversion was obtained after 24h with Au0.5Pd0.5 (85%) in comparison to Pd1 (36%). The effect of the both the reagents and products on the catalytic activity of the Au0.5Pd0.5 and Pd1 catalysts was evaluated using VTNA determining a Langmuir-Hinshelwood mechanism and differences in stability of both catalysts over time. The presence of Au in the AuPd NP in IL, leads to an increase in the robustness of the catalyst, increasing the H2 activation on the catalyst surface and decreasing the dependency on the [CAL] and [H2].
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spelling nottingham-647712023-11-15T13:33:27Z https://eprints.nottingham.ac.uk/64771/ Fabrication of AuPd bimetallic nanoparticles and their effects on hydrogenation reactions B. F. Pinto, Jose Jorge As catalytic reactions reach nearly 40 % of the world GDP, enhancing the catalytic properties of scarce metals, generating highly active, selective and durable catalysts is critical. Bimetallic AuPd NPs present enhanced activity and selectivity in hydrogenation reactions. However, the mechanisms behind their improved catalytic properties when compare to their monometallic counterparts and the enhancement effect of Au in the alloy remains ambiguous. This thesis elucidates the synergetic effect in AuPd NPs leading to their enhanced catalytic properties towards the selective hydrogenation of CAL. The AuPd NPs were first co-deposited in IL ([C4C1Im][NTf2]) by magnetron sputtering and their structural and electronic properties characterised. Evidence of the interaction of both metals with the disruption of the Au surface plasmon resonance in the presence of Pd (UV-vis) was observed and the absence of the Au-IL interaction with the increase of Pd content (XPS). XAS experiments confirmed the presence of a core-shell structure in the AuPd NPs with the preferential interaction of the SO2 groups in the IL anion with the sputtered Pd atoms leading to an ordering of the NP structure during growth and nucleation. Highest conversion was obtained after 24h with Au0.5Pd0.5 (85%) in comparison to Pd1 (36%). The effect of the both the reagents and products on the catalytic activity of the Au0.5Pd0.5 and Pd1 catalysts was evaluated using VTNA determining a Langmuir-Hinshelwood mechanism and differences in stability of both catalysts over time. The presence of Au in the AuPd NP in IL, leads to an increase in the robustness of the catalyst, increasing the H2 activation on the catalyst surface and decreasing the dependency on the [CAL] and [H2]. 2021-07-31 Thesis (University of Nottingham only) NonPeerReviewed application/pdf en cc_by https://eprints.nottingham.ac.uk/64771/1/Jos%C3%A9%20Jorge%20Pinto%20%5B14246470%5D%20correction%20version%20PhD%20thesis.pdf B. F. Pinto, Jose Jorge (2021) Fabrication of AuPd bimetallic nanoparticles and their effects on hydrogenation reactions. PhD thesis, University of Nottingham. Catalysis Nanoparticles Magnetron Sputtering
spellingShingle Catalysis
Nanoparticles
Magnetron Sputtering
B. F. Pinto, Jose Jorge
Fabrication of AuPd bimetallic nanoparticles and their effects on hydrogenation reactions
title Fabrication of AuPd bimetallic nanoparticles and their effects on hydrogenation reactions
title_full Fabrication of AuPd bimetallic nanoparticles and their effects on hydrogenation reactions
title_fullStr Fabrication of AuPd bimetallic nanoparticles and their effects on hydrogenation reactions
title_full_unstemmed Fabrication of AuPd bimetallic nanoparticles and their effects on hydrogenation reactions
title_short Fabrication of AuPd bimetallic nanoparticles and their effects on hydrogenation reactions
title_sort fabrication of aupd bimetallic nanoparticles and their effects on hydrogenation reactions
topic Catalysis
Nanoparticles
Magnetron Sputtering
url https://eprints.nottingham.ac.uk/64771/