Insight into the Thermodynamics of Graphene Growth on Copper

Paul Leidinger, Sebastian Günther

Research output: Contribution to journalArticlepeer-review

6 Scopus citations

Abstract

High-precision thermodynamic data were derived for single-layer graphene growth on Cu by measuring an increase or decrease in graphene flake size during chemical vapor deposition (CVD) in a reactive CH4/H2 atmosphere. An immediate flake shape change was observed when crossing the thermodynamic equilibrium of graphene formation, which was used as a sensitive criterion when systematically varying the CVD parameters during growth at 975-1080 °C. Extraction of the reaction enthalpy (ΔRH° = 91.8 ± 2.4 kJ·mol-1) and entropy (ΔRS° = 108.0 ± 1.8 J·mol-1·K-1) provides the anchoring point highly needed for calibration of experimental reactor studies or theoretical work. Comparing the Gibbs free energy with the thermodynamic data of graphite formation verifies that self-limiting single-layer graphene growth on copper occurs purely kinetically. Thermodynamics always favors the formation of multilayer graphene. Identifying the CVD parameter space where multilayer graphene is formed while single-layer graphene decays will foster the development of future synthesis strategies. The gained knowledge is transferable to other CVD-based graphene growth systems.

Original languageEnglish
Pages (from-to)12663-12671
Number of pages9
JournalJournal of Physical Chemistry C
Volume125
Issue number23
DOIs
StatePublished - 17 Jun 2021
Externally publishedYes

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