A comparative study of mechanisms of the adsorption of CO2 confined within graphene–MoS2 nanosheets: a DFT trend study

The space within the interlayer of 2-dimensional (2D) nanosheets provides new and intriguing confined environments for molecular interactions. However, atomic level understanding of the adsorption mechanism of CO2 confined within the interlayer of 2D nanosheets is still limited. Herein, we present a...

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Main Authors: Enujekwu, Francis M., Ezeh, Collins I., George, Michael W., Xu, Mengxia, Do, Hainam, Zhang, Yue, Zhao, Haitao, Wu, Tao
Format: Article
Language:English
Published: Royal Society of Chemistry 2019
Subjects:
Online Access:https://eprints.nottingham.ac.uk/56276/
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author Enujekwu, Francis M.
Ezeh, Collins I.
George, Michael W.
Xu, Mengxia
Do, Hainam
Zhang, Yue
Zhao, Haitao
Wu, Tao
author_facet Enujekwu, Francis M.
Ezeh, Collins I.
George, Michael W.
Xu, Mengxia
Do, Hainam
Zhang, Yue
Zhao, Haitao
Wu, Tao
author_sort Enujekwu, Francis M.
building Nottingham Research Data Repository
collection Online Access
description The space within the interlayer of 2-dimensional (2D) nanosheets provides new and intriguing confined environments for molecular interactions. However, atomic level understanding of the adsorption mechanism of CO2 confined within the interlayer of 2D nanosheets is still limited. Herein, we present a comparative study of the adsorption mechanisms of CO2 confined within graphene–molybdenum disulfide (MoS2) nanosheets using density functional theory (DFT). A comprehensive analysis of CO2 adsorption energies (EAE) at various interlayer spacings of different multilayer structures comprising graphene/graphene (GrapheneB) and MoS2/MoS2 (MoS2B) bilayers as well as graphene/MoS2 (GMoS2) and MoS2/graphene (MoS2G) hybrids is performed to obtain the most stable adsorption configurations. It was found that 7.5 Å and 8.5 Å interlayer spacings are the most stable conformations for CO2 adsorption on the bilayer and hybrid structures, respectively. Adsorption energies of the multilayer structures decreased in the following trend: MoS2B > GrapheneB > MoS2G > GMoS2. By incorporating van der Waals (vdW) interactions between the CO2 molecule and the surfaces, we find that CO2 binds more strongly on these multilayer structures. Furthermore, there is a slight discrepancy in the binding energies of CO2 adsorption on the heterostructures (GMoS2, MoS2G) due to the modality of the atom arrangement (C–Mo–S–O and Mo–S–O–C) in both structures, indicating that conformational anisotropy determines to a certain degree its CO2 adsorption energy. Meanwhile, Bader charge analysis shows that the interaction between CO2 and these surfaces causes charge transfer and redistributions. By contrast, the density of states (DOS) plots show that CO2 physisorption does not have a substantial effect on the electronic properties of graphene and MoS2. In summary, the results obtained in this study could serve as useful guidance in the preparation of graphene–MoS2 nanosheets for the improved adsorption efficiency of CO2.
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spelling nottingham-562762019-03-12T07:17:37Z https://eprints.nottingham.ac.uk/56276/ A comparative study of mechanisms of the adsorption of CO2 confined within graphene–MoS2 nanosheets: a DFT trend study Enujekwu, Francis M. Ezeh, Collins I. George, Michael W. Xu, Mengxia Do, Hainam Zhang, Yue Zhao, Haitao Wu, Tao The space within the interlayer of 2-dimensional (2D) nanosheets provides new and intriguing confined environments for molecular interactions. However, atomic level understanding of the adsorption mechanism of CO2 confined within the interlayer of 2D nanosheets is still limited. Herein, we present a comparative study of the adsorption mechanisms of CO2 confined within graphene–molybdenum disulfide (MoS2) nanosheets using density functional theory (DFT). A comprehensive analysis of CO2 adsorption energies (EAE) at various interlayer spacings of different multilayer structures comprising graphene/graphene (GrapheneB) and MoS2/MoS2 (MoS2B) bilayers as well as graphene/MoS2 (GMoS2) and MoS2/graphene (MoS2G) hybrids is performed to obtain the most stable adsorption configurations. It was found that 7.5 Å and 8.5 Å interlayer spacings are the most stable conformations for CO2 adsorption on the bilayer and hybrid structures, respectively. Adsorption energies of the multilayer structures decreased in the following trend: MoS2B > GrapheneB > MoS2G > GMoS2. By incorporating van der Waals (vdW) interactions between the CO2 molecule and the surfaces, we find that CO2 binds more strongly on these multilayer structures. Furthermore, there is a slight discrepancy in the binding energies of CO2 adsorption on the heterostructures (GMoS2, MoS2G) due to the modality of the atom arrangement (C–Mo–S–O and Mo–S–O–C) in both structures, indicating that conformational anisotropy determines to a certain degree its CO2 adsorption energy. Meanwhile, Bader charge analysis shows that the interaction between CO2 and these surfaces causes charge transfer and redistributions. By contrast, the density of states (DOS) plots show that CO2 physisorption does not have a substantial effect on the electronic properties of graphene and MoS2. In summary, the results obtained in this study could serve as useful guidance in the preparation of graphene–MoS2 nanosheets for the improved adsorption efficiency of CO2. Royal Society of Chemistry 2019-01-14 Article PeerReviewed application/pdf en cc_by_nc https://eprints.nottingham.ac.uk/56276/1/A%20Comparative%20Study%20of%20Mechanisms%20of%20the%20Adsorption%20of%20CO2%20Confined%20within%20Graphene-MoS2%20Nanosheets%20A%20DFT%20Trend%20Study%20-%20Published%20version.pdf Enujekwu, Francis M., Ezeh, Collins I., George, Michael W., Xu, Mengxia, Do, Hainam, Zhang, Yue, Zhao, Haitao and Wu, Tao (2019) A comparative study of mechanisms of the adsorption of CO2 confined within graphene–MoS2 nanosheets: a DFT trend study. Nanoscale Advances . ISSN 2516-0230 Adsorption mechanisms; density functional theory (DFT); graphene–MoS2 nanosheets; CO2 http://dx.doi.org/10.1039/C8NA00314A doi:10.1039/C8NA00314A doi:10.1039/C8NA00314A
spellingShingle Adsorption mechanisms; density functional theory (DFT); graphene–MoS2 nanosheets; CO2
Enujekwu, Francis M.
Ezeh, Collins I.
George, Michael W.
Xu, Mengxia
Do, Hainam
Zhang, Yue
Zhao, Haitao
Wu, Tao
A comparative study of mechanisms of the adsorption of CO2 confined within graphene–MoS2 nanosheets: a DFT trend study
title A comparative study of mechanisms of the adsorption of CO2 confined within graphene–MoS2 nanosheets: a DFT trend study
title_full A comparative study of mechanisms of the adsorption of CO2 confined within graphene–MoS2 nanosheets: a DFT trend study
title_fullStr A comparative study of mechanisms of the adsorption of CO2 confined within graphene–MoS2 nanosheets: a DFT trend study
title_full_unstemmed A comparative study of mechanisms of the adsorption of CO2 confined within graphene–MoS2 nanosheets: a DFT trend study
title_short A comparative study of mechanisms of the adsorption of CO2 confined within graphene–MoS2 nanosheets: a DFT trend study
title_sort comparative study of mechanisms of the adsorption of co2 confined within graphene–mos2 nanosheets: a dft trend study
topic Adsorption mechanisms; density functional theory (DFT); graphene–MoS2 nanosheets; CO2
url https://eprints.nottingham.ac.uk/56276/
https://eprints.nottingham.ac.uk/56276/
https://eprints.nottingham.ac.uk/56276/