Abstract

The role of the Mo2C/oxide interface on multi-layer graphene (MLG) nucleation during a chemical vapor deposition (CVD) process is investigated. During the CVD process, MLG growth is only observed in the presence of a Mo2C/SiO2 interface, indicating that the chemical reactions occurring at this interface trigger the nucleation of MLG. The chemical reaction pathway is explained in four steps as (1) creation of H radicals, (2) reduction of the oxide surface, (3) formation of C–C bonds at O–H sites, and (4) expansion of graphitic domains on the Mo2C catalyst. Different Mo2C/oxide interfaces are investigated, with varying affinity for reduction in a hydrogen environment. The results demonstrate a catalyst/oxide bifunctionality on MLG nucleation, comprising of CH4 dehydrogenation by Mo2C and initial C–C bond formation at the oxide interface.

Highlights

  • The role of the ­Mo2C/oxide interface on multi-layer graphene (MLG) nucleation during a chemical vapor deposition (CVD) process is investigated

  • We will test this model by performing the CVD process in absence of hydrogen gas, as well as using different oxide (­ TiO2, ­Al2O3, MgO) interfaces, in which we expect a dependence of MLG nucleation on the oxide reducibility

  • The outcome of this study shows that the catalyst-oxide interface interaction is crucial for understanding the MLG synthesis on ­Mo2C thin films

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Summary

Introduction

The role of the ­Mo2C/oxide interface on multi-layer graphene (MLG) nucleation during a chemical vapor deposition (CVD) process is investigated. ­Mo2C in combination with ZSM-5 zeolite supports causes aromatization of ­CH4, whereas this is not the case for only ­Mo2C or ZSM-5 ­separately[23] This shows that both the catalyst and neighboring oxide can play a role in graphene synthesis, which to our knowledge has not yet been investigated. We will introduce a model for explaining the MLG nucleation by catalyst/ oxide bi-functionality This model is based on the complementary role of MoCx (x = 0–0.5) for ­CH4 dehydrogenation and ­SiO2 for C–C bond formation after reduction with hydrogen. We will test this model by performing the CVD process in absence of hydrogen gas, as well as using different oxide (­ TiO2, ­Al2O3, MgO) interfaces, in which we expect a dependence of MLG nucleation on the oxide reducibility. The outcome of this study shows that the catalyst-oxide interface interaction is crucial for understanding the MLG synthesis on ­Mo2C thin films

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