Catalytic Performance Of Multi-Component Copper-Based Catalyst For Direct Carbon Dioxide Hydrogenation To Methanol

Methanol production from direct CO2 hydrogenation is a useful strategy to utilize CO2 and a practical approach to sustainable development. Improving the efficiency of the reaction is crucial for encouraging the decentralize of the technology and this is achievable via the development of active catal...

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Main Author:	Koh, Mei Kee
Format:	Thesis
Language:	English
Published:	2018
Subjects:	T Technology TP155-156 Chemical engineering
Online Access:	http://eprints.usm.my/47775/1/Catalytic%20Performance%20Of%20Multi-Component%20Copper-Based%20Catalyst%20For%20Direct%20Carbon%20Dioxide%20Hydrogenation%20To%20Methanol.pdf
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spelling	my-usm-ep.477752021-11-17T03:42:13Z Catalytic Performance Of Multi-Component Copper-Based Catalyst For Direct Carbon Dioxide Hydrogenation To Methanol 2018-09-01 Koh, Mei Kee T Technology TP155-156 Chemical engineering Methanol production from direct CO2 hydrogenation is a useful strategy to utilize CO2 and a practical approach to sustainable development. Improving the efficiency of the reaction is crucial for encouraging the decentralize of the technology and this is achievable via the development of active catalysts. After rigorous screenings, multi-component 0.6Cu/0.15ZnO/0.05MnO/1.0SBA-15 (CZM/SBA-15) was developed in this study. The introduction of SBA-15 as catalyst support effectively improved the catalyst texture. The addition of MnO as promoter created strong interactions between CuO and other oxide species in the catalyst. Besides, MnO also promoted the formation of small copper crystallites. In this way, the hydrogen adsorption capacity of the catalyst was enhanced, leading to strong hydrogenation strength. A moderate interaction between CZM/SBA-15 and CO2 molecules was found crucial for enhancing CO2 conversion. The methanol selectivity was remarkably increased to more than 90% due to the availability of metal-oxide(s) interfacial area to stabilize reaction intermediates. Then, the morphological impact of porous supports on copper crystallites and effective diffusivity (catalyst pore-geometry dependent coefficient) of catalyst were investigated. The porous supports selected for investigation were SBA-15, MCF and KIT-6. Among all, KIT-6 supported catalyst (CZM/KIT-6) presented the most superior properties. The morphology of KIT-6 deterred mesopore plugging and favoured the formation of small copper crystallites. CZM/KIT-6 also possessed greater resistance to copper crystallite growth and loss of copper surface area during reaction due to the pore-confining effect of the porous support and the larger inter-crystallite spacing between copper crystallites. The high effective diffusivity of CZM/KIT-6 enhanced the transfer of reactant molecules to active sites and the removal of reaction products. Next, the effect of weight-hourly space velocity (WHSV, 8-120 L/gcat.h), reaction temperature (160-260°C) and pressure (1.0-5.0 MPa) on the performance of CZM/KIT-6 were investigated. The response of CO2 conversion and methanol selectivity to these parameters strictly obey the reaction thermodynamic. In stability study, the performance of CZM/KIT-6 during 120 h time-on-stream was maintained at high level. Compared to the pre-reduced catalyst, the copper crystallite growth of CZM/KIT-6 spent in the stability experiment was 50.7% and the loss of copper surface area was 33.9%. On the average, the CO2 conversion attained was 27.6% and the methanol selectivity was 88.3%. The average methanol yield was 24.4% and this corresponds to methanol formation rate of 71.6 mol/kgcat.h. 2018-09 Thesis http://eprints.usm.my/47775/ http://eprints.usm.my/47775/1/Catalytic%20Performance%20Of%20Multi-Component%20Copper-Based%20Catalyst%20For%20Direct%20Carbon%20Dioxide%20Hydrogenation%20To%20Methanol.pdf application/pdf en public phd doctoral Universiti Sains Malaysia Pusat Pengajian Kejuruteraan Kimia
institution	Universiti Sains Malaysia
collection	USM Institutional Repository
language	English
topic	T Technology TP155-156 Chemical engineering
spellingShingle	T Technology TP155-156 Chemical engineering Koh, Mei Kee Catalytic Performance Of Multi-Component Copper-Based Catalyst For Direct Carbon Dioxide Hydrogenation To Methanol
description	Methanol production from direct CO2 hydrogenation is a useful strategy to utilize CO2 and a practical approach to sustainable development. Improving the efficiency of the reaction is crucial for encouraging the decentralize of the technology and this is achievable via the development of active catalysts. After rigorous screenings, multi-component 0.6Cu/0.15ZnO/0.05MnO/1.0SBA-15 (CZM/SBA-15) was developed in this study. The introduction of SBA-15 as catalyst support effectively improved the catalyst texture. The addition of MnO as promoter created strong interactions between CuO and other oxide species in the catalyst. Besides, MnO also promoted the formation of small copper crystallites. In this way, the hydrogen adsorption capacity of the catalyst was enhanced, leading to strong hydrogenation strength. A moderate interaction between CZM/SBA-15 and CO2 molecules was found crucial for enhancing CO2 conversion. The methanol selectivity was remarkably increased to more than 90% due to the availability of metal-oxide(s) interfacial area to stabilize reaction intermediates. Then, the morphological impact of porous supports on copper crystallites and effective diffusivity (catalyst pore-geometry dependent coefficient) of catalyst were investigated. The porous supports selected for investigation were SBA-15, MCF and KIT-6. Among all, KIT-6 supported catalyst (CZM/KIT-6) presented the most superior properties. The morphology of KIT-6 deterred mesopore plugging and favoured the formation of small copper crystallites. CZM/KIT-6 also possessed greater resistance to copper crystallite growth and loss of copper surface area during reaction due to the pore-confining effect of the porous support and the larger inter-crystallite spacing between copper crystallites. The high effective diffusivity of CZM/KIT-6 enhanced the transfer of reactant molecules to active sites and the removal of reaction products. Next, the effect of weight-hourly space velocity (WHSV, 8-120 L/gcat.h), reaction temperature (160-260°C) and pressure (1.0-5.0 MPa) on the performance of CZM/KIT-6 were investigated. The response of CO2 conversion and methanol selectivity to these parameters strictly obey the reaction thermodynamic. In stability study, the performance of CZM/KIT-6 during 120 h time-on-stream was maintained at high level. Compared to the pre-reduced catalyst, the copper crystallite growth of CZM/KIT-6 spent in the stability experiment was 50.7% and the loss of copper surface area was 33.9%. On the average, the CO2 conversion attained was 27.6% and the methanol selectivity was 88.3%. The average methanol yield was 24.4% and this corresponds to methanol formation rate of 71.6 mol/kgcat.h.
format	Thesis
qualification_name	Doctor of Philosophy (PhD.)
qualification_level	Doctorate
author	Koh, Mei Kee
author_facet	Koh, Mei Kee
author_sort	Koh, Mei Kee
title	Catalytic Performance Of Multi-Component Copper-Based Catalyst For Direct Carbon Dioxide Hydrogenation To Methanol
title_short	Catalytic Performance Of Multi-Component Copper-Based Catalyst For Direct Carbon Dioxide Hydrogenation To Methanol
title_full	Catalytic Performance Of Multi-Component Copper-Based Catalyst For Direct Carbon Dioxide Hydrogenation To Methanol
title_fullStr	Catalytic Performance Of Multi-Component Copper-Based Catalyst For Direct Carbon Dioxide Hydrogenation To Methanol
title_full_unstemmed	Catalytic Performance Of Multi-Component Copper-Based Catalyst For Direct Carbon Dioxide Hydrogenation To Methanol
title_sort	catalytic performance of multi-component copper-based catalyst for direct carbon dioxide hydrogenation to methanol
granting_institution	Universiti Sains Malaysia
granting_department	Pusat Pengajian Kejuruteraan Kimia
publishDate	2018
url	http://eprints.usm.my/47775/1/Catalytic%20Performance%20Of%20Multi-Component%20Copper-Based%20Catalyst%20For%20Direct%20Carbon%20Dioxide%20Hydrogenation%20To%20Methanol.pdf
_version_	1747821828747821056

Catalytic Performance Of Multi-Component Copper-Based Catalyst For Direct Carbon Dioxide Hydrogenation To Methanol

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