Structure and chemistry of graphene oxide in liquid water from first principles

Abstract

Graphene oxide is a rising star among 2D materials, yet its interaction with liquid water remains a fundamentally open question: experimental characterization at the atomic scale is difficult, and modeling by classical approaches cannot properly describe chemical reactivity. Here, we bridge the gap between simple computational models and complex experimental systems, by realistic first-principles molecular simulations of graphene oxide (GO) in liquid water. We construct chemically accurate GO models and study their behavior in water, showing that oxygen-bearing functional groups (hydroxyl and epoxides) are preferentially clustered on the graphene oxide layer. We demonstrated the specific properties of GO in water, an unusual combination of both hydrophilicity and fast water dynamics. Finally, we evidence that GO is chemically active in water, acquiring an average negative charge of the order of 10 mC m −2 . The ab initio modeling highlights the uniqueness of GO structures for applications as innovative membranes for desalination and water purification.

Full text

Its licence does not allow us to show the full text. Read it at PubMed Central:

References 63

1. 1.

   Dreyer DR, Park S, Bielawski CW, Ruoff RS. The chemistry of graphene oxide. Chem. Soc. Rev. 2010;39:228-240.

   Not in our library10.1039/b917103g

2. 2.

   Zhu Y, et al. Graphene and graphene oxide: synthesis, properties, and applications. Adv. Mater. 2010;22:3906-3924.

   Not in our library10.1002/adma.201001068

3. 3.

   Joshi RK, et al. Precise and ultrafast molecular sieving through graphene oxide membranes. Science. 2014;343:752-754.

   Not in our library10.1126/science.1245711

4. 4.

   Su Y, et al. Impermeable barrier films and protective coatings based on reduced graphene oxide. Nat. Commun. 2014;5:3906.

   Not in our library10.1038/ncomms4906

5. 5.

   Kumar S, et al. Graphene oxide–MnFe2O4 magnetic nanohybrids for efficient removal of lead and arsenic from water. ACS Appl. Mater. Interfaces. 2014;6:17426-17436.

   Not in our library10.1021/am504826q

6. 6.

   Favaro M, et al. Multiple doping of graphene oxide foams and quantum dots: new switchable systems for oxygen reduction and water remediation. J. Mater. Chem. A. 2015;3:14334-14347.

   Not in our library10.1039/c5ta01561h

7. 7.

   Dutta D, Thiyagarajan S, Bahadur D. SnO2 quantum dots decorated reduced graphene oxide nanocomposites for efficient water remediation. Chem. Eng. J. 2016;297:55-65.

   Not in our library10.1016/j.cej.2016.03.130

8. 8.

   Yadav R, Subhash A, Chemmenchery N, Kandasubramanian B. Graphene and graphene oxide for fuel cell technology. Ind. Eng. Chem. Res. 2018;57:9333-9350.

   Not in our library10.1021/acs.iecr.8b02326

9. 9.

   Farooqui U, Ahmad A, Hamid N. Graphene oxide: a promising membrane material for fuel cells. Renew. Sustain. Energy Rev. 2018;82:714-733.

   Not in our library10.1016/j.rser.2017.09.081

10. 10.

    Nakajima T, Mabuchi A, Hagiwara R. A new structure model of graphite oxide. Carbon. 1988;26:357-361.

    Not in our library10.1016/0008-6223(88)90227-8

11. 11.

    Szabó T, et al. Evolution of surface functional groups in a series of progressively oxidized graphite oxides. Chem. Mater. 2006;18:2740-2749.

    Not in our library10.1021/cm060258+

12. 12.

    Stankovich S, Piner RD, Nguyen ST, Ruoff RS. Synthesis and exfoliation of isocyanate-treated graphene oxide nanoplatelets. Carbon. 2006;44:3342-3347.

    Not in our library10.1016/j.carbon.2006.06.004

13. 13.

    Stankovich S, et al. Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide. Carbon. 2007;45:1558-1565.

    Not in our library10.1016/j.carbon.2007.02.034

14. 14.

    Yang D, et al. Chemical analysis of graphene oxide films after heat and chemical treatments by X-ray photoelectron and micro-raman spectroscopy. Carbon. 2009;47:145-152.

    Not in our library10.1016/j.carbon.2008.09.045

15. 15.

    Schniepp HC, et al. Functionalized single graphene sheets derived from splitting graphite oxide. J. Phys. Chem. B. 2006;110:8535-8539.

    Not in our library10.1021/jp060936f

16. 16.

    McAllister MJ, et al. Single sheet functionalized graphene by oxidation and thermal expansion of graphite. Chem. Mater. 2007;19:4396-4404.

    Not in our library10.1021/cm0630800

17. 17.

    He H, Klinowski J, Forster M, Lerf A. A new structural model for graphite oxide. Chem. Phys. Lett. 1998;287:53-56.

    Not in our library10.1016/s0009-2614(98)00144-4

18. 18.

    Lerf A, He H, Forster M, Klinowski J. Structure of graphite oxide revisited. J. Phys. Chem. B. 1998;102:4477-4482.

    Not in our library10.1021/jp9731821

19. 19.

    Yan J-A, Xian L, Chou MY. Structural and electronic properties of oxidized graphene. Phys. Rev. Lett. 2009;103:086802.

    Not in our library10.1103/physrevlett.103.086802

20. 20.

    Lee DW, et al. The structure of graphite oxide: Investigation of its surface chemical groups. J. Phys. Chem. B. 2010;114:5723-5728.

    Not in our library10.1021/jp1002275

21. 21.

    Bagri A, et al. Structural evolution during the reduction of chemically derived graphene oxide. Nat. Chem. 2010;2:581-587.

    Not in our library10.1038/nchem.686

22. 22.

    Wei N, Peng X, Xu Z. Understanding water permeation in graphene oxide membranes. ACS Appl. Mater. Interfaces. 2014;6:5877-5883.

    Not in our library10.1021/am500777b

23. 23.

    Devanathan R, Chase-Woods D, Shin Y, Gotthold DW. Molecular dynamics simulations reveal that water diffusion between graphene oxide layers is slow. Sci. Rep. 2016;6:457.

    Not in our library10.1038/srep29484

24. 24.

    Cohen-Tanugi D, Lin L-C, Grossman JC. Multilayer nanoporous graphene membranes for water desalination. Nano Lett. 2016;16:1027-1033.

    Not in our library10.1021/acs.nanolett.5b04089

25. 25.

    Hou D, Yang T. A reactive molecular dynamics study of graphene oxide sheets in different saturated states: structure, reactivity and mechanical properties. Phys. Chem. Chem. Phys. 2018;20:11053-11066.

    Not in our library10.1039/c8cp00813b

26. 26.

    Cassagneau T, Guérin F, Fendler JH. Preparation and characterization of ultrathin films layer-by-layer self-assembled from graphite oxide nanoplatelets and polymers. Langmuir. 2000;16:7318-7324.

    Not in our library10.1021/la000442o

27. 27.

    Boukhvalov DW, Katsnelson MI. Modeling of graphite oxide. J. Am. Chem. Soc. 2008;130:10697-10701.

    Not in our library10.1021/ja8021686

28. 28.

    Yang Q, et al. Ultrathin graphene-based membrane with precise molecular sieving and ultrafast solvent permeation. Nat. Mater. 2017;16:1198-1202.

    Not in our library10.1038/nmat5025

29. 29.

    Zhou K-G, et al. Electrically controlled water permeation through graphene oxide membranes. Nature. 2018;559:236-240.

    Not in our library10.1038/s41586-018-0292-y

30. 30.

    Kudin KN, et al. Raman spectra of graphite oxide and functionalized graphene sheets. Nano Lett. 2008;8:36-41.

    Not in our library10.1021/nl071822y

31. 31.

    Yan J-A, Chou MY. Oxidation functional groups on graphene: structural and electronic properties. Phys. Rev. B. 2010;82:17.

    Not in our library

32. 32.

    Wang B, Bocquet M-L, Marchini S, Günther S, Wintterlin J. Chemical origin of a graphene Moiré overlayer on Ru(0001). Phys. Chem. Chem. Phys. 2008;10:3530-3534.

    Not in our library10.1039/b801785a

33. 33.

    Wang B, Bocquet M-L, Günther S, Wintterlin J. Comment on “Periodically rippled graphene: growth and spatially resolved electronic structure”. Phys. Rev. Lett. 2008;101:099703.

    Not in our library10.1103/physrevlett.101.099703

34. 34.

    Zhou S, Bongiorno A. Origin of the chemical and kinetic stability of graphene oxide. Sci Rep. 2013;3:457.

    Not in our library10.1038/srep02484

35. 35.

    Kumar PV, et al. New insights into the thermal reduction of graphene oxide: impact of oxygen clustering. Carbon. 2016;100:90-98.

    Not in our library10.1016/j.carbon.2015.12.087

36. 36.

    Xia S, Ni M, Zhu T, Zhao Y, Li N. Ultrathin graphene oxide nanosheet membranes with various d-spacing assembled using the pressure-assisted filtration method for removing natural organic matter. Desalination. 2015;371:78-87.

    Not in our library10.1016/j.desal.2015.06.005

37. 37.

    Abraham J, et al. Tunable sieving of ions using graphene oxide membranes. Nat. Nanotechnol. 2017;12:546-550.

    Not in our library10.1038/nnano.2017.21

38. 38.

    Khoei AR, Khorrami MS. Mechanical properties of graphene oxide: a molecular dynamics study. Fuller. Nanotub. Carbon Nanostruct. 2016;24:594-603.

    Not in our library10.1080/1536383x.2016.1208180

39. 39.

    Fraux, G. Chemfiles, available online at https://zenodo.org/record/3490304#.Xab2mS3M1QI.

    Not in our library

40. 40.

    Fraux, G. cfiles, available online at https://github.com/chemfiles/cfiles.

    Not in our library

Cited by papers we hold 1

• Multifunctional GelMA platforms with nanomaterials for advanced tissue therapeutics · 2022
  No notice

Reads

A person counts once a day per paper. We keep no cookie and no address: a reader is a hash that changes every day. Any month under five reads shows no number.