A molecular understanding of the gas-phase reduction and doping of graphene oxide
),
Xinran Wang1(
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Chemical reduction of graphene oxide represents an important route towards large-scale production of graphene sheets for many applications. Thus far, gas-phase reactions have been demonstrated to efficiently reduce graphene oxide, but a molecular understanding of the reaction processes is largely lacking. Here, using molecular dynamics simulations, we compare the reduction of graphene oxide in different environments. We find that NH3 affords more efficient reduction of hydroxyl and epoxide groups than H2 and vacuum annealing partly due to lower energy barriers. Various reduction paths of oxygen groups in NH3 and H2 are quantitatively identified. Furthermore, we show that with the combination of vacancies and oxygen groups, pyridinic- or pyrrolic-like nitrogen can readily be incorporated into graphene. All of these nitrogen configurations lead to n-doping of the graphene. Our results are consistent with many previous experiments and provide insights towards doping engineering of graphene.
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A molecular understanding of the gas-phase reduction and doping of graphene oxide
), Xinran Wang1(
)
Abstract
Chemical reduction of graphene oxide represents an important route towards large-scale production of graphene sheets for many applications. Thus far, gas-phase reactions have been demonstrated to efficiently reduce graphene oxide, but a molecular understanding of the reaction processes is largely lacking. Here, using molecular dynamics simulations, we compare the reduction of graphene oxide in different environments. We find that NH3 affords more efficient reduction of hydroxyl and epoxide groups than H2 and vacuum annealing partly due to lower energy barriers. Various reduction paths of oxygen groups in NH3 and H2 are quantitatively identified. Furthermore, we show that with the combination of vacancies and oxygen groups, pyridinic- or pyrrolic-like nitrogen can readily be incorporated into graphene. All of these nitrogen configurations lead to n-doping of the graphene. Our results are consistent with many previous experiments and provide insights towards doping engineering of graphene.
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Acknowledgements
We thank Prof. J. Dong for helpful discussions. This work was partially supported by the National Science and Technology Major Project (No. 2011ZX02707), the Chinese National Key Fundamental Research Project (Nos. 2011CB922103 and 2007CB936300), and the National Natural Science Foundation of China (Nos. 60990314, 61076017 and 60928009).
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