Comparing Ultralong Carbon Nanotube Growth from Methane over Mono- and Bi-Metallic Iron Chloride Catalysts

Yick, Tim; Gangoli, Varun; White, Alvin Orbaek

doi:10.3390/nano13152172

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Comparing Ultralong Carbon Nanotube Growth from Methane over Mono- and Bi-Metallic Iron Chloride Catalysts

Tim Yick, Varun Gangoli

, Alvin Orbaek White

Nanomaterials, Volume: 13, Issue: 15, Start page: 2172

Swansea University Authors: Tim Yick, Varun Gangoli , Alvin Orbaek White

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DOI (Published version): 10.3390/nano13152172

Abstract

This research endeavours to study the growth of ultralong carbon nanotubes (UL-CNTs) from methane using diverse catalysts, namely FeCl3, bi-metallic Fe-Cu, Fe-Ni, and Fe-Co chlorides. Aqueous catalyst solutions were evenly dispersed on silica substrates and grown at 950 °C in the presence of hydroge...

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Published in:	Nanomaterials
ISSN:	2079-4991
Published:	MDPI AG 2023
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URI:	https://cronfa.swan.ac.uk/Record/cronfa64117
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Aqueous catalyst solutions were evenly dispersed on silica substrates and grown at 950 °C in the presence of hydrogen via a horizontal chemical vapour deposition (CVD) furnace. The samples underwent characterisation by Raman spectroscopy, scanning electron microscopy (SEM), and optical microscopy to identify the quality of CNTs and enumerate individual UL-CNTs. Our findings revealed that FeCl3, as a mono-metallic catalyst, generated the longest UL-CNTs, which measured 1.32 cm, followed by Fe-Cu (0.85 cm), Fe-Co (0.7 cm), and Fe-Ni (0.6 cm), respectively. The G/D ratio (graphene to defects) from the Raman spectroscopy was the highest with the FeCl3 catalyst (3.09), followed by Fe-Cu (2.79), Fe-Co catalyst (2.13), and Fe-Ni (2.52). It indicates that the mono-iron-based catalyst also produces the highest purity CNTs. Moreover, this study scrutinises the vapour-liquid-solid (VLS) model for CNT growth and the impact of carbide formation as a precursor to CNT growth. Our research findings indicate that forming iron carbide (Fe3C) is a crucial transition phase for amorphous carbon transformation to CNTs. Notably, the iron catalyst generated the longest and densest CNTs relative to other iron-based bi-metallic catalysts, which is consistent with the temperature of carbide formation in the mono-metallic system. From correlations made using the phase diagram with carbon, we conclude that CNT growth is favoured because of increased carbon solubility within the mono-metallic catalyst compared to the bi-metallic catalysts.</abstract><type>Journal Article</type><journal>Nanomaterials</journal><volume>13</volume><journalNumber>15</journalNumber><paginationStart>2172</paginationStart><paginationEnd/><publisher>MDPI AG</publisher><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint/><issnElectronic>2079-4991</issnElectronic><keywords>carbon nanotube; ultralong carbon nanotube; iron chloride; vapour-liquid-solid</keywords><publishedDay>26</publishedDay><publishedMonth>6</publishedMonth><publishedYear>2023</publishedYear><publishedDate>2023-06-26</publishedDate><doi>10.3390/nano13152172</doi><url>http://dx.doi.org/10.3390/nano13152172</url><notes/><college>COLLEGE NANME</college><department>Science and Engineering - Faculty</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>FGSEN</DepartmentCode><institution>Swansea University</institution><apcterm>Another institution paid the OA fee</apcterm><funders>A.O.W. was funded through the Sêr Cymru II Fellowship by the Welsh Government and the European Regional Development Fund (ERDF). A.O.W. and T.Y. acknowledge funding from the Welsh Government Circular Economy Capital Fund for FY 2020–21. V.S.G. is funded thanks to Salts Healthcare Ltd. and TRIMTABS Ltd. The authors acknowledge access to the SEM provided by the Swansea University AIM Facility, funded partly by the EPSRC (EP/M028267/1), the European Regional Development Fund through the Welsh Government (80708), and the Welsh Government’s Sêr Cymru program.</funders><projectreference/><lastEdited>2023-10-02T11:52:20.5944966</lastEdited><Created>2023-08-23T15:03:28.1533479</Created><path><level id="1">Faculty of Science and Engineering</level><level id="2">School of Engineering and Applied Sciences - Uncategorised</level></path><authors><author><firstname>Tim</firstname><surname>Yick</surname><order>1</order></author><author><firstname>Varun</firstname><surname>Gangoli</surname><orcid>0000-0001-5313-5839</orcid><order>2</order></author><author><firstname>Alvin</firstname><surname>Orbaek White</surname><order>3</order></author></authors><documents><document><filename>64117__28361__8d54c6e4e3bc4b5e8d231bec693f6936.pdf</filename><originalFilename>64117.pdf</originalFilename><uploaded>2023-08-23T15:06:48.3873195</uploaded><type>Output</type><contentLength>5093116</contentLength><contentType>application/pdf</contentType><version>Version of Record</version><cronfaStatus>true</cronfaStatus><documentNotes>This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license.</documentNotes><copyrightCorrect>true</copyrightCorrect><language>eng</language><licence>https://creativecommons.org/licenses/by/4.0/</licence></document></documents><OutputDurs/></rfc1807>
spelling	v2 64117 2023-08-23 Comparing Ultralong Carbon Nanotube Growth from Methane over Mono- and Bi-Metallic Iron Chloride Catalysts ccb07360981496ff88079701bd101801 Tim Yick Tim Yick true false 677b4758fd9d95755d516b096be7d396 0000-0001-5313-5839 Varun Gangoli Varun Gangoli true false 8414a23650d4403fdfe1a735dbd2e24e Alvin Orbaek White Alvin Orbaek White true false 2023-08-23 FGSEN This research endeavours to study the growth of ultralong carbon nanotubes (UL-CNTs) from methane using diverse catalysts, namely FeCl3, bi-metallic Fe-Cu, Fe-Ni, and Fe-Co chlorides. Aqueous catalyst solutions were evenly dispersed on silica substrates and grown at 950 °C in the presence of hydrogen via a horizontal chemical vapour deposition (CVD) furnace. The samples underwent characterisation by Raman spectroscopy, scanning electron microscopy (SEM), and optical microscopy to identify the quality of CNTs and enumerate individual UL-CNTs. Our findings revealed that FeCl3, as a mono-metallic catalyst, generated the longest UL-CNTs, which measured 1.32 cm, followed by Fe-Cu (0.85 cm), Fe-Co (0.7 cm), and Fe-Ni (0.6 cm), respectively. The G/D ratio (graphene to defects) from the Raman spectroscopy was the highest with the FeCl3 catalyst (3.09), followed by Fe-Cu (2.79), Fe-Co catalyst (2.13), and Fe-Ni (2.52). It indicates that the mono-iron-based catalyst also produces the highest purity CNTs. Moreover, this study scrutinises the vapour-liquid-solid (VLS) model for CNT growth and the impact of carbide formation as a precursor to CNT growth. Our research findings indicate that forming iron carbide (Fe3C) is a crucial transition phase for amorphous carbon transformation to CNTs. Notably, the iron catalyst generated the longest and densest CNTs relative to other iron-based bi-metallic catalysts, which is consistent with the temperature of carbide formation in the mono-metallic system. From correlations made using the phase diagram with carbon, we conclude that CNT growth is favoured because of increased carbon solubility within the mono-metallic catalyst compared to the bi-metallic catalysts. Journal Article Nanomaterials 13 15 2172 MDPI AG 2079-4991 carbon nanotube; ultralong carbon nanotube; iron chloride; vapour-liquid-solid 26 6 2023 2023-06-26 10.3390/nano13152172 http://dx.doi.org/10.3390/nano13152172 COLLEGE NANME Science and Engineering - Faculty COLLEGE CODE FGSEN Swansea University Another institution paid the OA fee A.O.W. was funded through the Sêr Cymru II Fellowship by the Welsh Government and the European Regional Development Fund (ERDF). A.O.W. and T.Y. acknowledge funding from the Welsh Government Circular Economy Capital Fund for FY 2020–21. V.S.G. is funded thanks to Salts Healthcare Ltd. and TRIMTABS Ltd. The authors acknowledge access to the SEM provided by the Swansea University AIM Facility, funded partly by the EPSRC (EP/M028267/1), the European Regional Development Fund through the Welsh Government (80708), and the Welsh Government’s Sêr Cymru program. 2023-10-02T11:52:20.5944966 2023-08-23T15:03:28.1533479 Faculty of Science and Engineering School of Engineering and Applied Sciences - Uncategorised Tim Yick 1 Varun Gangoli 0000-0001-5313-5839 2 Alvin Orbaek White 3 64117__28361__8d54c6e4e3bc4b5e8d231bec693f6936.pdf 64117.pdf 2023-08-23T15:06:48.3873195 Output 5093116 application/pdf Version of Record true This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license. true eng https://creativecommons.org/licenses/by/4.0/
title	Comparing Ultralong Carbon Nanotube Growth from Methane over Mono- and Bi-Metallic Iron Chloride Catalysts
spellingShingle	Comparing Ultralong Carbon Nanotube Growth from Methane over Mono- and Bi-Metallic Iron Chloride Catalysts Tim Yick Varun Gangoli Alvin Orbaek White
title_short	Comparing Ultralong Carbon Nanotube Growth from Methane over Mono- and Bi-Metallic Iron Chloride Catalysts
title_full	Comparing Ultralong Carbon Nanotube Growth from Methane over Mono- and Bi-Metallic Iron Chloride Catalysts
title_fullStr	Comparing Ultralong Carbon Nanotube Growth from Methane over Mono- and Bi-Metallic Iron Chloride Catalysts
title_full_unstemmed	Comparing Ultralong Carbon Nanotube Growth from Methane over Mono- and Bi-Metallic Iron Chloride Catalysts
title_sort	Comparing Ultralong Carbon Nanotube Growth from Methane over Mono- and Bi-Metallic Iron Chloride Catalysts
author_id_str_mv	ccb07360981496ff88079701bd101801 677b4758fd9d95755d516b096be7d396 8414a23650d4403fdfe1a735dbd2e24e
author_id_fullname_str_mv	ccb07360981496ff88079701bd101801_*_Tim Yick 677b4758fd9d95755d516b096be7d396__Varun Gangoli 8414a23650d4403fdfe1a735dbd2e24e_**_Alvin Orbaek White
author	Tim Yick Varun Gangoli Alvin Orbaek White
author2	Tim Yick Varun Gangoli Alvin Orbaek White
format	Journal article
container_title	Nanomaterials
container_volume	13
container_issue	15
container_start_page	2172
publishDate	2023
institution	Swansea University
issn	2079-4991
doi_str_mv	10.3390/nano13152172
publisher	MDPI AG
college_str	Faculty of Science and Engineering
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hierarchy_top_title	Faculty of Science and Engineering
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hierarchy_parent_title	Faculty of Science and Engineering
department_str	School of Engineering and Applied Sciences - Uncategorised{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Uncategorised
url	http://dx.doi.org/10.3390/nano13152172
document_store_str	1
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description	This research endeavours to study the growth of ultralong carbon nanotubes (UL-CNTs) from methane using diverse catalysts, namely FeCl3, bi-metallic Fe-Cu, Fe-Ni, and Fe-Co chlorides. Aqueous catalyst solutions were evenly dispersed on silica substrates and grown at 950 °C in the presence of hydrogen via a horizontal chemical vapour deposition (CVD) furnace. The samples underwent characterisation by Raman spectroscopy, scanning electron microscopy (SEM), and optical microscopy to identify the quality of CNTs and enumerate individual UL-CNTs. Our findings revealed that FeCl3, as a mono-metallic catalyst, generated the longest UL-CNTs, which measured 1.32 cm, followed by Fe-Cu (0.85 cm), Fe-Co (0.7 cm), and Fe-Ni (0.6 cm), respectively. The G/D ratio (graphene to defects) from the Raman spectroscopy was the highest with the FeCl3 catalyst (3.09), followed by Fe-Cu (2.79), Fe-Co catalyst (2.13), and Fe-Ni (2.52). It indicates that the mono-iron-based catalyst also produces the highest purity CNTs. Moreover, this study scrutinises the vapour-liquid-solid (VLS) model for CNT growth and the impact of carbide formation as a precursor to CNT growth. Our research findings indicate that forming iron carbide (Fe3C) is a crucial transition phase for amorphous carbon transformation to CNTs. Notably, the iron catalyst generated the longest and densest CNTs relative to other iron-based bi-metallic catalysts, which is consistent with the temperature of carbide formation in the mono-metallic system. From correlations made using the phase diagram with carbon, we conclude that CNT growth is favoured because of increased carbon solubility within the mono-metallic catalyst compared to the bi-metallic catalysts.
published_date	2023-06-26T11:52:23Z
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Comparing Ultralong Carbon Nanotube Growth from Methane over Mono- and Bi-Metallic Iron Chloride Catalysts

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