Cyclodehydrogenation of molecular nanographene precursors catalyzed by atomic hydrogen

Abstract Atomically precise synthesis of graphene nanostructures on semiconductors and insulators has been a formidable challenge. In particular, the metallic substrates needed to catalyze cyclodehydrogenative planarization reactions limit subsequent applications that exploit the electronic and/or m...

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Main Authors: Rafal Zuzak, Pawel Dabczynski, Jesús Castro-Esteban, José Ignacio Martínez, Mads Engelund, Dolores Pérez, Diego Peña, Szymon Godlewski
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-54774-1
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author Rafal Zuzak
Pawel Dabczynski
Jesús Castro-Esteban
José Ignacio Martínez
Mads Engelund
Dolores Pérez
Diego Peña
Szymon Godlewski
author_facet Rafal Zuzak
Pawel Dabczynski
Jesús Castro-Esteban
José Ignacio Martínez
Mads Engelund
Dolores Pérez
Diego Peña
Szymon Godlewski
author_sort Rafal Zuzak
collection DOAJ
description Abstract Atomically precise synthesis of graphene nanostructures on semiconductors and insulators has been a formidable challenge. In particular, the metallic substrates needed to catalyze cyclodehydrogenative planarization reactions limit subsequent applications that exploit the electronic and/or magnetic structure of graphene derivatives. Here, we introduce a protocol in which an on-surface reaction is initiated and carried out regardless of the substrate type. We demonstrate that, counterintuitively, atomic hydrogen can play the role of a catalyst in the cyclodehydrogenative planarization reaction. The high efficiency of the method is demonstrated by the nanographene synthesis on metallic Au, semiconducting TiO2, Ge:H, as well as on inert and insulating Si/SiO2 and thin NaCl layers. The hydrogen-catalyzed cyclodehydrogenation reaction reported here leads towards the integration of graphene derivatives in optoelectronic devices as well as developing the field of on-surface synthesis by means of catalytic transformations. It also inspires merging of atomically shaped graphene-based nanostructures with low-dimensional inorganic units into functional devices.
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institution Kabale University
issn 2041-1723
language English
publishDate 2025-01-01
publisher Nature Portfolio
record_format Article
series Nature Communications
spelling doaj-art-8335326ce8f04f4e97ca914338b124402025-01-19T12:32:03ZengNature PortfolioNature Communications2041-17232025-01-0116111010.1038/s41467-024-54774-1Cyclodehydrogenation of molecular nanographene precursors catalyzed by atomic hydrogenRafal Zuzak0Pawel Dabczynski1Jesús Castro-Esteban2José Ignacio Martínez3Mads Engelund4Dolores Pérez5Diego Peña6Szymon Godlewski7Faculty of Physics, Astronomy and Applied Computer Science, Jagiellonian UniversityFaculty of Physics, Astronomy and Applied Computer Science, Jagiellonian UniversityCentro de Investigación en Química Biolóxica e Materiais Moleculares (CiQUS) and Departamento de Química Orgánica, Universidade de Santiago de CompostelaInstituto de Ciencia de Materiales de Madrid, Consejo Superior de Investigaciones Científicas (ICMM-CSIC)Espeem S.A.R.L. (espeem.com)Centro de Investigación en Química Biolóxica e Materiais Moleculares (CiQUS) and Departamento de Química Orgánica, Universidade de Santiago de CompostelaCentro de Investigación en Química Biolóxica e Materiais Moleculares (CiQUS) and Departamento de Química Orgánica, Universidade de Santiago de CompostelaFaculty of Physics, Astronomy and Applied Computer Science, Jagiellonian UniversityAbstract Atomically precise synthesis of graphene nanostructures on semiconductors and insulators has been a formidable challenge. In particular, the metallic substrates needed to catalyze cyclodehydrogenative planarization reactions limit subsequent applications that exploit the electronic and/or magnetic structure of graphene derivatives. Here, we introduce a protocol in which an on-surface reaction is initiated and carried out regardless of the substrate type. We demonstrate that, counterintuitively, atomic hydrogen can play the role of a catalyst in the cyclodehydrogenative planarization reaction. The high efficiency of the method is demonstrated by the nanographene synthesis on metallic Au, semiconducting TiO2, Ge:H, as well as on inert and insulating Si/SiO2 and thin NaCl layers. The hydrogen-catalyzed cyclodehydrogenation reaction reported here leads towards the integration of graphene derivatives in optoelectronic devices as well as developing the field of on-surface synthesis by means of catalytic transformations. It also inspires merging of atomically shaped graphene-based nanostructures with low-dimensional inorganic units into functional devices.https://doi.org/10.1038/s41467-024-54774-1
spellingShingle Rafal Zuzak
Pawel Dabczynski
Jesús Castro-Esteban
José Ignacio Martínez
Mads Engelund
Dolores Pérez
Diego Peña
Szymon Godlewski
Cyclodehydrogenation of molecular nanographene precursors catalyzed by atomic hydrogen
Nature Communications
title Cyclodehydrogenation of molecular nanographene precursors catalyzed by atomic hydrogen
title_full Cyclodehydrogenation of molecular nanographene precursors catalyzed by atomic hydrogen
title_fullStr Cyclodehydrogenation of molecular nanographene precursors catalyzed by atomic hydrogen
title_full_unstemmed Cyclodehydrogenation of molecular nanographene precursors catalyzed by atomic hydrogen
title_short Cyclodehydrogenation of molecular nanographene precursors catalyzed by atomic hydrogen
title_sort cyclodehydrogenation of molecular nanographene precursors catalyzed by atomic hydrogen
url https://doi.org/10.1038/s41467-024-54774-1
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