Ammonia adsorption on graphene and graphene oxide: a first-principles study

doi:10.1007/s11783-013-0491-6

Front Envir Sci Eng

2013, Vol. 7

Issue (3) : 403-411 https://doi.org/10.1007/s11783-013-0491-6

RESEARCH ARTICLE

Ammonia adsorption on graphene and graphene oxide: a first-principles study

Yue PENG, Junhua LI(

)

State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China

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Abstract

Motivated by the recent realization of graphene sensor to detect gas molecules that are harmful to the environment, the ammonia adsorption on graphene or graphene oxide (GO) was investigated using first-principles calculation. The optimal adsorption and orientation of the NH₃ molecules on the graphene surfaces were determined, and the adsorption energies (E_b) as well as the Mulliken charge transfers of NH₃ were calculated. The E_b for the graphene are small and seem to be independent of the sites and orientations. The surface epoxy or hydroxyl groups can promote the adsorption of NH₃ on the GO; the enhancement of the E_b for the hydroxyl groups is greater than that for the epoxy groups on the surface. The charge transfers from the molecule to the surfaces also exhibit the same trend. The Br?nsted acid sites and Lewis acid sites could stably exist on the GO with surface hydroxyl groups and on the basal, respectively.

Keywords graphene oxide first-principles calculations NH₃ adsorption

Corresponding Author(s): LI Junhua,Email:lijunhua@tsinghua.edu.cn

Issue Date: 01 June 2013

Cite this article:

Yue PENG,Junhua LI. Ammonia adsorption on graphene and graphene oxide: a first-principles study[J]. Front Envir Sci Eng, 2013, 7(3): 403-411.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-013-0491-6
https://academic.hep.com.cn/fese/EN/Y2013/V7/I3/403

Fig.1 Schematic representation of graphene

Fig.2 Optimized NH adsorption on graphene. The order is in accordance with sequence order of Table 1

Tab.1 Adsorption on graphene: the binding energy (), the charge transfer () from molecule to graphene for the different configurations

Fig.3 Schematic representation of GO with epoxy groups in a carbon hexagon: (a) C-O-C; (b) C-OO-C; (c) C-O_O-C; and (d) C-O__O-C

Fig.4 Optimized NH adsorption on GO with epoxy groups in a carbon hexagon. The order is in accordance with sequence order of Table 2

Tab.2 Adsorption on GO with epoxy groups

Fig.5 Schematic representation of GO with hydroxyl groups in a carbon hexagon: (a) C-OH and (b) C-OH__HO-C

Fig.6 Optimized NH adsorption on GO with hydrogen groups in a carbon hexagon. The order is in accordance with sequence order of Table 3

Tab.3 Adsorption on GO with hydroxyl groups

Fig.7 Schematic representation of GO with epoxy and hydrogen groups in a carbon hexagon: (a) C-OOH and (b) C-O_OH

Fig.8 Optimized NH adsorption on GO with epoxy and hydrogen groups in a carbon hexagon. The order is in accordance with sequence order of Table 4

Tab.4 Adsorption on GO with epoxy and hydroxyl groups

Fig.9 Schematic representation of GO with epoxy or hydrogen groups on the basal: (a) C-OOH(op); (b) C-OH__OH-C(op); (c) C-OO-C(op)

Fig.10 Optimized NH adsorption on GO with epoxy and hydrogen groups on the basal. The order is in accordance with sequence order of Table 5

Tab.5 Adsorption on GO with epoxy and hydroxyl groups on the basal

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