Scaled‐Up Graphene Growth Through Chemical Vapor Deposition Over Large‐Area Liquid Cu Catalysts
Abstract This study scales up the chemical vapor deposition (CVD) process for graphene growth using CH₄ and H₂ mixtures on large molten Cu substrates using a liquid metal catalyst (LMCat) reactor. In situ optical microscopy and ex situ Raman spectroscopy reveal key differences from previous studies...
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| Main Authors: | , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley-VCH
2025-06-01
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| Series: | Advanced Materials Interfaces |
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| Online Access: | https://doi.org/10.1002/admi.202401005 |
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| author | Mahesh K. Prabhu Christos Tsakonas Yilei Tian Marc deVoogd Kees E. Kolmeijer Anastasios Manikas Gertjan vanBaarle Grégory F. Schneider Costas Galiotis Irene M. N. Groot |
| author_facet | Mahesh K. Prabhu Christos Tsakonas Yilei Tian Marc deVoogd Kees E. Kolmeijer Anastasios Manikas Gertjan vanBaarle Grégory F. Schneider Costas Galiotis Irene M. N. Groot |
| author_sort | Mahesh K. Prabhu |
| collection | DOAJ |
| description | Abstract This study scales up the chemical vapor deposition (CVD) process for graphene growth using CH₄ and H₂ mixtures on large molten Cu substrates using a liquid metal catalyst (LMCat) reactor. In situ optical microscopy and ex situ Raman spectroscopy reveal key differences from previous studies on smaller molten Cu surfaces. Graphene grown on large molten Cu exhibits improved quality and uniformity at low [CH₄]/[H₂] ratios. A shift in the growth mechanism is observed: at low [CH₄]/[H₂], single‐front growth yields high‐quality graphene, whereas higher ratios cause multiple nuclei to merge, forming a nucleation‐flow‐merger pattern. Raman spectroscopy confirms uniform graphene quality at low [CH₄]/[H₂]. At intermediate [CH₄]/[H₂], few‐layer graphene grows uniformly on larger Cu substrates. Finite element analysis using COMSOL Multiphysics shows that efficient heating of reaction gases by molten Cu enhances graphene growth. An empirical model, developed from experimental data, reliably predicts the fastest graphene growth on large liquid Cu substrates. These findings address critical challenges and advance the feasibility of continuous, industrial‐scale graphene production using molten metal catalysts. |
| format | Article |
| id | doaj-art-36b7a3ea4b4043f4b43c2fed489fe53f |
| institution | OA Journals |
| issn | 2196-7350 |
| language | English |
| publishDate | 2025-06-01 |
| publisher | Wiley-VCH |
| record_format | Article |
| series | Advanced Materials Interfaces |
| spelling | doaj-art-36b7a3ea4b4043f4b43c2fed489fe53f2025-08-20T02:34:04ZengWiley-VCHAdvanced Materials Interfaces2196-73502025-06-011211n/an/a10.1002/admi.202401005Scaled‐Up Graphene Growth Through Chemical Vapor Deposition Over Large‐Area Liquid Cu CatalystsMahesh K. Prabhu0Christos Tsakonas1Yilei Tian2Marc deVoogd3Kees E. Kolmeijer4Anastasios Manikas5Gertjan vanBaarle6Grégory F. Schneider7Costas Galiotis8Irene M. N. Groot9Leiden Institute of Chemistry Leiden University Einsteinweg 55 Leiden 2333 CC The NetherlandsFORTH/ICE‐HT and Department of Chemical Engineering University of Patras Patras 26504 GreeceLeiden Probe Microscopy Kenauweg 21 Leiden 2331 BA The NetherlandsLeiden Probe Microscopy Kenauweg 21 Leiden 2331 BA The NetherlandsLeiden Institute of Chemistry Leiden University Einsteinweg 55 Leiden 2333 CC The NetherlandsFORTH/ICE‐HT and Department of Chemical Engineering University of Patras Patras 26504 GreeceLeiden Probe Microscopy Kenauweg 21 Leiden 2331 BA The NetherlandsLeiden Institute of Chemistry Leiden University Einsteinweg 55 Leiden 2333 CC The NetherlandsFORTH/ICE‐HT and Department of Chemical Engineering University of Patras Patras 26504 GreeceLeiden Institute of Chemistry Leiden University Einsteinweg 55 Leiden 2333 CC The NetherlandsAbstract This study scales up the chemical vapor deposition (CVD) process for graphene growth using CH₄ and H₂ mixtures on large molten Cu substrates using a liquid metal catalyst (LMCat) reactor. In situ optical microscopy and ex situ Raman spectroscopy reveal key differences from previous studies on smaller molten Cu surfaces. Graphene grown on large molten Cu exhibits improved quality and uniformity at low [CH₄]/[H₂] ratios. A shift in the growth mechanism is observed: at low [CH₄]/[H₂], single‐front growth yields high‐quality graphene, whereas higher ratios cause multiple nuclei to merge, forming a nucleation‐flow‐merger pattern. Raman spectroscopy confirms uniform graphene quality at low [CH₄]/[H₂]. At intermediate [CH₄]/[H₂], few‐layer graphene grows uniformly on larger Cu substrates. Finite element analysis using COMSOL Multiphysics shows that efficient heating of reaction gases by molten Cu enhances graphene growth. An empirical model, developed from experimental data, reliably predicts the fastest graphene growth on large liquid Cu substrates. These findings address critical challenges and advance the feasibility of continuous, industrial‐scale graphene production using molten metal catalysts.https://doi.org/10.1002/admi.2024010052D materialCVDempirical modelgraphenehigh qualitylarge area |
| spellingShingle | Mahesh K. Prabhu Christos Tsakonas Yilei Tian Marc deVoogd Kees E. Kolmeijer Anastasios Manikas Gertjan vanBaarle Grégory F. Schneider Costas Galiotis Irene M. N. Groot Scaled‐Up Graphene Growth Through Chemical Vapor Deposition Over Large‐Area Liquid Cu Catalysts Advanced Materials Interfaces 2D material CVD empirical model graphene high quality large area |
| title | Scaled‐Up Graphene Growth Through Chemical Vapor Deposition Over Large‐Area Liquid Cu Catalysts |
| title_full | Scaled‐Up Graphene Growth Through Chemical Vapor Deposition Over Large‐Area Liquid Cu Catalysts |
| title_fullStr | Scaled‐Up Graphene Growth Through Chemical Vapor Deposition Over Large‐Area Liquid Cu Catalysts |
| title_full_unstemmed | Scaled‐Up Graphene Growth Through Chemical Vapor Deposition Over Large‐Area Liquid Cu Catalysts |
| title_short | Scaled‐Up Graphene Growth Through Chemical Vapor Deposition Over Large‐Area Liquid Cu Catalysts |
| title_sort | scaled up graphene growth through chemical vapor deposition over large area liquid cu catalysts |
| topic | 2D material CVD empirical model graphene high quality large area |
| url | https://doi.org/10.1002/admi.202401005 |
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