Document Type : Original research
Authors
1 Department of Polymer Engineering and Color Technology, Amirkabir University of Technology, Tehran, Iran
2 New Technologies Research Center (NTRC), Amirkabir University of Technology, Tehran, Iran
Abstract
The effect of structural defects on graphene interaction with other molecules is of high interest. In this study, the interaction of ethylene molecules with pristine graphene (PG) and defective graphenes including single (SVG) and double (DVG) vacancies, were investigated using dispersion-corrected periodic density functional theory (DFT). We used various pairs of pseudopotentials and dispersion-corrected methods to calculate the exchange-correlation energies and long-range energies, respectively. We conducted the calculations in the ethylene-graphene equilibrium distance where vdW interaction as a long-range interaction was dominant. Both adsorption and deformation energies were calculated to examine the possibility of ethylene chemisorption. It was found that there is a critical distance from the graphene surface, where the nature of adsorption of adsorbate molecule changes from physisorption to the possible chemisorption depending on the energetical costly distortion induced in adsorbate molecule. In the case of ethylene adsorption on the graphene structures studied here, the mentioned critical distances follow the order SVG < DVG < PG. However, in the range of vdW domination and in comparison with PG, ethylene interacts more with SVG due to the presence of a dangling bond and interacts less with DVG due to the presence of a hole. Furthermore, the interactions of ethylene with reconstructed trivacancy were studied. Moreover, all possible orientations for ethylene adsorption on graphene structures were considered and energetically compared. All calculations were done on fully optimized reconstructed geometries of vacancies with structural characteristics, i.e., reconstruction length and formation energies comparable to those reported in the literature.
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- Novoselov KS, Geim AK, Morozov SV, Jiang D-E, Zhang Y, Dubonos SV, Grigorieva IV, Firsov AA (2004) Electric field effect in atomically thin carbon films. Science 306: 666-669
- Navalon S, Dhakshinamoorthy A, Alvaro M, Garcia H (2014) Carbocatalysis by graphene-based materials. Chem Rev 114: 6179-6212
- Fan X, Zhang G, Zhang F (2015) Multiple roles of graphene in heterogeneous catalysis. Chem Soc Rev 44: 3023-3035
- Antonietti M, Navalón S, Dhakshinamoorthy A, Álvaro M, García H (2018) Carbocatalysis: Analyzing the sources of organic transformations. In: Carbon-based metal-free catalysts: Design and applications 1, 285-311
- Nag A, Mitra A, Mukhopadhyay SC (2018) Graphene and its sensor-based applications: A review. Sens Actuator A Phys 270: 177-194
- Liu G, Jin W, Xu N (2015) Graphene-based membranes. Chem Soc Rev 44: 5016-5030
- Gao Y, Neal L, Ding D, Wu W, Baroi C, Gaffney AM, Li F (2019) Recent advances in intensified ethylene production-A review. ACS Catal 9: 8592-8621
- Primo A, Neatu F, Florea M, Parvulescu V, Garcia H (2014) Graphenes in the absence of metals as carbocatalysts for selective acetylene hydrogenation and alkene hydrogenation. Nat commun 5: 5291
- Perhun TI, Bychko IB, Trypolsky AI, Strizhak PE (2013) Catalytic properties of graphene material in the hydrogenation of ethylene. Theor Exp Chem 48: 367-370
- Abakumov AA, Bychko IB, Nikolenko AS, Strizhak PE (2018) Catalytic activity of n-doped reduced graphene oxide in the hydrogenation of ethylene and acetylene. Theor Exp Chem 54: 218-224
- Zhang X, Kumari G, Heo J, Jain PK (2018) In situ formation of catalytically active graphene in ethylene photo-epoxidation. Nat Commun 9: 3056
- Chang J, Zhang Y, Yao Y, Liu X, Hildebrandt D (2022) Reduced graphene oxide supported cobalt catalysts for ethylene hydroformylation: Modified cobalt-support interaction by rhodium. Fuel 324: 124479
- Liu X, Yang Y, Chu M, Duan T, Meng C, Han Y (2016) Defect stabilized gold atoms on graphene as potential catalysts for ethylene epoxidation: A first-principles investigation. Catal Sci Technol 6: 1632-1641
- Navalon S, Dhakshinamoorthy A, Alvaro M, Antonietti M, García H (2017) Active sites on graphene-based materials as metal-free catalysts. Chem Soc Rev
- Stephan DW, Erker G (2010) Frustrated Lewis pairs: Metal-free hydrogen activation and more. Angew Chem Int Ed 49: 46-76
- Sastre G, Forneli A, Almasan V, Parvulescu VI, Garcia H (2017) Isotopic h/d exchange on graphenes. A combined experimental and theoretical study. Appl Catal 547: 52-59
- Lee JS, Ko YS (2014) Synthesis of petaloid graphene/polyethylene composite nanosheet produced by ethylene polymerization with metallocene catalyst adsorbed on multilayer graphene. Catal Today 232: 82-88
- Nia AS, Binder WH (2017) Graphene as initiator/catalyst in polymerization chemistry. Prog Polym Sci 67: 48-76
- Zhang H-X, Ko E-B, Park J-H, Moon Y-K, Zhang X-Q, Yoon K-B (2016) Fabrication of polyethylene/graphene nanocomposites through in situ polymerization with a spherical graphene/ MgCl2-supported Ziegler-Natta catalyst. Compos Sci Technol 136: 61-66
- Kheradmand A, Ramazani Sa A, Khorasheh F, Baghalha M, Bahrami H (2015) Effects of nano graphene oxide as support on the product properties and performance of Ziegler–Natta catalyst in production of UHMWPE. Polym Adv Technol 26: 315-321
- Zhang H, Park J-H, Moon Y-K, Ko E-B, Lee D-H, Hu Y, Zhang X, Yoon K-B (2017) Preparation of graphene/MgCl2-supported Ti-based Ziegler-Natta catalysts by the coagglomeration method and their application in ethylene polymerization. Chinese J Catal 38: 131- 137
- Chmutin I, Novokshonova L, Brevnov P, Yukhayeva G, Ryvkina N (2017) Electrical properties of UHMWPE/graphite nanoplates composites obtained by in-situ polymerization method. Polyolefins J 4: 1-12
- Abdolahzadeh T, Morshedian J, Ahmadi S (2022) Preparation and characterization of nano WO3/ Bi2O3/GO and BaSO4/GO dispersed HDPE composites for X-ray shielding application. Polyolefins J 9: 73-83
- Shehzad F, Daud M, Al-Harthi MA (2016) Synthesis, characterization and crystallization kinetics of nanocomposites prepared by in situ polymerization of ethylene and graphene. J Therm Anal 123: 1501-1511
- Li K, Li N, Yan N, Wang T, Zhang Y, Song Q, Li H (2020) Adsorption of small hydrocarbons on pristine, n-doped and vacancy graphene by DFT study. Appl Surf Sci 515: 146028
- Wang C, Xiao B, Ding Y-H (2013) Theoretical investigation on the healing mechanism of divacancy defect in graphene growth by reaction with ethylene and acetylene. New J Chem 37: 640-645
- Kokalj A (2022) Corrosion inhibitors: Physisorbed or chemisorbed? Corros Sci 196: 109939
- Giannozzi P, Baroni S, Bonini N, Calandra M, Car R, Cavazzoni C, Ceresoli D, Chiarotti GL, Cococcioni M, Dabo I (2009) Quantum espresso: A modular and open-source software project for quantum simulations of materials. J Phys Condens 21: 395502
- Giannozzi P, Andreussi O, Brumme T, Bunau O, Nardelli MB, Calandra M, Car R, Cavazzoni C, Ceresoli D, Cococcioni M (2017) Advanced capabilities for materials modelling with quantum espresso. J Phys Condens 29: 465901
- Monkhorst HJ, Pack JD (1976) Special points for brillouin-zone integrations. Phys Rev B 13: 5188
- Perdew JP, Burke K, Ernzerhof M (1996) Generalized gradient approximation made simple. Phys Rev lett 77: 3865
- Perdew JP, Ruzsinszky A, Csonka GI, Vydrov OA, Scuseria GE, Constantin LA, Zhou X, Burke K (2008) Restoring the density-gradient expansion for exchange in solids and surfaces. Phys Rev lett 100: 136406
- Grimme S, Antony J, Ehrlich S, Krieg H (2010) A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-d) for the 94 elements H-Pu. Chem Phys 132: 154104
- Skowron ST, Lebedeva IV, Popov AM, Bichoutskaia E (2015) Energetics of atomic scale structure changes in graphene. Chem Soc Rev 44: 3143-3176
- Robertson AW, Lee G-D, He K, Yoon E, Kirkland AI, Warner JH (2014) The role of the bridging atom in stabilizing odd numbered graphene vacancies. Nano Lett 14: 3972-3980
- Yamashita K, Saito M, Oda T (2006) Atomic geometry and stability of mono-, di-, and trivacancies in graphene. Jpn J Appl Phys 45: 6534
- Kotakoski J, Meyer J, Kurasch S, Santos-Cottin D, Kaiser U, Krasheninnikov A (2011) Stone-wales-type transformations in carbon nanostructures driven by electron irradiation. Phys Rev B 83: 245420
- GüRel HH, Ozçelik VO, Ciraci S (2014) Dissociative adsorption of molecules on graphene and silicene. Phys Chem C 118: 27574-27582