High-Quality Graphene Using Boudouard Reaction

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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
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Advanced Science, Volume 9, issue 12
Following the game-changing high-pressure CO (HiPco) process that established the first facile route toward large-scale production of single-walled carbon nanotubes, CO synthesis of cm-sized graphene crystals of ultra-high purity grown during tens of minutes is proposed. The Boudouard reaction serves for the first time to produce individual monolayer structures on the surface of a metal catalyst, thereby providing a chemical vapor deposition technique free from molecular and atomic hydrogen as well as vacuum conditions. This approach facilitates inhibition of the graphene nucleation from the CO/CO2 mixture and maintains a high growth rate of graphene seeds reaching large-scale monocrystals. Unique features of the Boudouard reaction coupled with CO-driven catalyst engineering ensure not only suppression of the second layer growth but also provide a simple and reliable technique for surface cleaning. Aside from being a novel carbon source, carbon monoxide ensures peculiar modification of catalyst and in generalopens avenues for breakthrough graphene-catalyst composite production.
Funding Information: The authors thank Mr. Andrei Starkov for illustrations and Mrs. Anastasiya Grebenko for assistance with sample synthesis. This work was performed using equipment of MIPT Shared Facilities Center. The authors acknowledge Vadim Khrapai and Evgeny Tikhonov (ISSP) for assistance with low temperature measurements and professor Galina Tsirlina (MSU) for fruitful discussions. The authors are also grateful to Salavat Khasanov for assistance and verification of XRD measurements. The authors thank the Helmholtz‐Zentrum Berlin für Materialien und Energie for the allocation of synchrotron radiation beamtime. Computations were done at the Finnish IT Center for Science, CSC. Russian Foundation for Basic Research grant # 19‐32‐90143 (A.K.G., A.G.N.). German Federal Ministry of Education and Research (BMBF) grant no. 05K19KER (A.A.M.). Russian Science Foundation No. 21‐19‐00226 (D.V.K., graphene synthesis). Russian Science Foundation No. 21‐72‐20050 (B.P.G., THz‐FIR spectroscopy). Ministry of Science and Higher Education of the Russian Federation within the governmental order for Boreskov Institute of Catalysis project АААА‐А21‐121011390011‐4 (A.N.S.). Partially supported by the Ministry of Science and Higher Education of the Russian Federation No. FSMG‐2021‐0005 (V.S.V., ARPES studies) and Russian Science Foundation No. 21‐72‐30026 (V.S.V, STM Studies). The work was supported by the Council on grants of the President of the Russian Federation grant number НШ‐1330.2022.1.3. Publisher Copyright: © 2022 The Authors. Advanced Science published by Wiley-VCH GmbH
Boudouard reaction, carbon monoxide, chemical vapor deposition, copper, graphene
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Grebenko , A K , Krasnikov , D V , Bubis , A V , Stolyarov , V S , Vyalikh , D V , Makarova , A A , Fedorov , A , Aitkulova , A , Alekseeva , A A , Gilshtein , E , Bedran , Z , Shmakov , A N , Alyabyeva , L , Mozhchil , R N , Ionov , A M , Gorshunov , B P , Laasonen , K , Podzorov , V & Nasibulin , A G 2022 , ' High-Quality Graphene Using Boudouard Reaction ' , Advanced Science , vol. 9 , no. 12 , 2200217 . https://doi.org/10.1002/advs.202200217