期刊
2D MATERIALS
卷 2, 期 2, 页码 -出版社
IOP PUBLISHING LTD
DOI: 10.1088/2053-1583/2/2/024008
关键词
graphene; functionalization; polycrystalline; grain boundary; oxidation; hydrogenation
资金
- Spanish Ministry of Economy and Competitiveness [MAT2012-33911]
- SAMSUNG Global Innovation Program
- Secretaria de Universidades e Investigacion del Departamento de Economia y Conocimiento de la Generalitat de Catalunya, from the Severo Ochoa Program [MINECO SEV-2013-0295]
- SECITI (Mexico)
- German Research Foundation (DFG) in the framework of the Priority Program 1459 'Graphene'
- Nanosystems Initiative Munich (NIM)
- European Union [280433, 604391]
- ICREA Funding Source: Custom
Grain boundaries, inevitably present in chemical vapor deposited graphene, are expected to have considerable impact on the development of graphene-based hybrid materials with tailored material properties. We demonstrate here the critical role of polycrystallinity on the chemical functionalization of graphene comparing ozone-induced oxidation with remote plasma hydrogenation. We show that graphene oxidation and hydrogenation occur in two consecutive stages upon increasing defect density: an initial step in which surface-bound functional groups are generated, followed by the creation of vacancies. Remarkably, we find that hydrogenation yields homogeneously distributed defects while ozone-induced defects are preferentially accumulated at the grain boundaries eventually provoking local cracking of the structure. Supported by quantum simulations, our experimental findings reveal distinct electronic transport regimes depending on the density and distribution of induced defects on the polycrystalline graphene films. Our findings highlight the key role played by grain boundaries during graphene functionalization, and at the same time provide a novel perspective to tailor the properties of polycrystalline graphene.
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