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Development of bimetallic Pd-Zn catalysts for methanol steam reforming: hydrogen production for fuel cells

Proton exchange membrane fuel cell (PEMFC) has been reported as clean and efficient energy technology from conversion of H₂. However, one of the main challenges remains the storage and transport of hydrogen. The promising alternative is to produce H₂ on site by a reformer using a H₂-dense liquid as...

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Main Author: Xalabile, Philasande
Other Authors: Fletcher, Jack
Format: Thesis
Language:English
Published: Centre for Catalysis Research 2017
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access_status_str Open Access
author Xalabile, Philasande
author2 Fletcher, Jack
author_browse Fletcher, Jack
Xalabile, Philasande
author_facet Fletcher, Jack
Xalabile, Philasande
author_sort Xalabile, Philasande
collection Thesis
description Proton exchange membrane fuel cell (PEMFC) has been reported as clean and efficient energy technology from conversion of H₂. However, one of the main challenges remains the storage and transport of hydrogen. The promising alternative is to produce H₂ on site by a reformer using a H₂-dense liquid as a fuel, a technology known as fuel processing. Methanol is an attractive source of H₂ compared to other fuels as it presents several advantages, i.e. it is obtained sulphur-free, has a high H to C ratio and therefore produces a H₂-rich reformate, can be reformed at low temperatures (200 - 300°C) and is a liquid at ambient conditions so that it can be easily handled. Typically, Cu-based catalysts are used for steam reforming of methanol due to their high activity (i.e. H₂ production) and high selectivity towards CO₂. As CO poisons anodic catalyst of PEMFC, high selectivity towards CO₂ is crucial so as to eliminate or at least minimize CO removal load downstream a fuel processor. However, Cubased catalysts are thermally unstable and suffer deactivation due to sintering at high temperatures (> 250°C). Moreover, Cu-based catalysts are pyrophoric and therefore difficult to handle. Recent studies show that PdZn catalysts are very promising as they exhibit comparable activity and selectivity to Cu-based ones. Furthermore, PdZn catalysts are thermally stable in the typically methanol steam reforming temperature range (200 - 300°C). Most literature attributes high CO₂ selectivity of PdZn catalysts to formation of PdZn alloy. It is generally agreed that PdZn alloy is formed when PdZn catalysts are reduced in H₂ at high temperatures (> 250°C). In this work, a Pd/ZnO catalyst aimed at 2.5 wt% Pd was successfully prepared via incipient wetness impregnation and the duplicate preparation of the catalyst was successful. Both impregnation catalysts were confirmed by ICP-OES to contain similar weight Pd loadings i.e. 2.8 and 2.7 wt%, respectively. The actual Pd loading (ICP-OES) was slightly higher than the target loading (2.5 wt%) due to Pd content of Pd salt underestimated during catalyst preparation. Furthermore, crystallite size distribution, i.e. PdO crystallites on ZnO support, was similar (i.e. 6.7 ± 2.4 nm and 6.3 ± 1.9 nm) for both impregnation catalysts.
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institution University of Cape Town (South Africa)
language eng
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license_str Not specified — see source repository
provenance_str_mv Harvested via OAI-PMH from UCTD — University of Cape Town Open Access Repository
publishDate 2017
publishDateRange 2017
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publisher Centre for Catalysis Research
publisherStr Centre for Catalysis Research
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source_str UCTD — University of Cape Town Open Access Repository
spelling oai:open.uct.ac.za:11427/24325 Development of bimetallic Pd-Zn catalysts for methanol steam reforming: hydrogen production for fuel cells Xalabile, Philasande Fletcher, Jack Luchters, Niels Malatji, Peter Catalysis Research Chemical Engineering Proton exchange membrane fuel cell (PEMFC) has been reported as clean and efficient energy technology from conversion of H₂. However, one of the main challenges remains the storage and transport of hydrogen. The promising alternative is to produce H₂ on site by a reformer using a H₂-dense liquid as a fuel, a technology known as fuel processing. Methanol is an attractive source of H₂ compared to other fuels as it presents several advantages, i.e. it is obtained sulphur-free, has a high H to C ratio and therefore produces a H₂-rich reformate, can be reformed at low temperatures (200 - 300°C) and is a liquid at ambient conditions so that it can be easily handled. Typically, Cu-based catalysts are used for steam reforming of methanol due to their high activity (i.e. H₂ production) and high selectivity towards CO₂. As CO poisons anodic catalyst of PEMFC, high selectivity towards CO₂ is crucial so as to eliminate or at least minimize CO removal load downstream a fuel processor. However, Cubased catalysts are thermally unstable and suffer deactivation due to sintering at high temperatures (> 250°C). Moreover, Cu-based catalysts are pyrophoric and therefore difficult to handle. Recent studies show that PdZn catalysts are very promising as they exhibit comparable activity and selectivity to Cu-based ones. Furthermore, PdZn catalysts are thermally stable in the typically methanol steam reforming temperature range (200 - 300°C). Most literature attributes high CO₂ selectivity of PdZn catalysts to formation of PdZn alloy. It is generally agreed that PdZn alloy is formed when PdZn catalysts are reduced in H₂ at high temperatures (> 250°C). In this work, a Pd/ZnO catalyst aimed at 2.5 wt% Pd was successfully prepared via incipient wetness impregnation and the duplicate preparation of the catalyst was successful. Both impregnation catalysts were confirmed by ICP-OES to contain similar weight Pd loadings i.e. 2.8 and 2.7 wt%, respectively. The actual Pd loading (ICP-OES) was slightly higher than the target loading (2.5 wt%) due to Pd content of Pd salt underestimated during catalyst preparation. Furthermore, crystallite size distribution, i.e. PdO crystallites on ZnO support, was similar (i.e. 6.7 ± 2.4 nm and 6.3 ± 1.9 nm) for both impregnation catalysts. 2017-05-16T08:01:22Z 2017-05-16T08:01:22Z 2015 Master Thesis Masters MSc (Eng) http://hdl.handle.net/11427/24325 eng application/pdf Centre for Catalysis Research Faculty of Engineering and the Built Environment University of Cape Town
spellingShingle Catalysis Research
Chemical Engineering
Xalabile, Philasande
Development of bimetallic Pd-Zn catalysts for methanol steam reforming: hydrogen production for fuel cells
thesis_degree_str Master's
title Development of bimetallic Pd-Zn catalysts for methanol steam reforming: hydrogen production for fuel cells
title_full Development of bimetallic Pd-Zn catalysts for methanol steam reforming: hydrogen production for fuel cells
title_fullStr Development of bimetallic Pd-Zn catalysts for methanol steam reforming: hydrogen production for fuel cells
title_full_unstemmed Development of bimetallic Pd-Zn catalysts for methanol steam reforming: hydrogen production for fuel cells
title_short Development of bimetallic Pd-Zn catalysts for methanol steam reforming: hydrogen production for fuel cells
title_sort development of bimetallic pd zn catalysts for methanol steam reforming hydrogen production for fuel cells
topic Catalysis Research
Chemical Engineering
url http://hdl.handle.net/11427/24325
work_keys_str_mv AT xalabilephilasande developmentofbimetallicpdzncatalystsformethanolsteamreforminghydrogenproductionforfuelcells