Smith, Andrew, Kelly, Nicole L., Figiel, Lukasz, Wan, Chaoying, Hanna, John V., Farris, Stefano and McNally, Tony (2020) Graphene-oxide functionalized with 2-Ureido-4[1H]-pyrimidinone for production of nacre-like films. ACS Applied Nano Materials . doi:10.1021/acsanm.0c01488 (In Press)

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Abstract

The facile and efficient reaction of graphene oxide (GO) and 2-Ureido-4[1H]-pyrimidinone (UPy), an isocyanate terminated 4-site hydrogen-bonding moiety, produces a functionalised GO (f-GO) that readily self-assembles into a freestanding nacre-like film using a vacuum filtration process. The reaction of UPy with GO occurs predominately via the epoxide and hydroxyl groups on the GO which was confirmed from a combination of Fourier-transform infrared (FTIR), Raman and X-ray photoelectron spectroscopy (XPS) and 13C Solid State Nuclear Magnetic Resonance (SSNMR) measurements. The nacre-like films obtained were typically 50µm to 100µm thick, from cross-section scanning-electron microscopy (SEM) imaging. The GO d-spacing (X-ray diffraction, XRD) increased with increasing UPy content from 0.934nm to 1.45nm, resulting in porous films with reduced tortuosity to oxygen, carbon dioxide and water. However, at higher UPy content reduced tortuosity is, balanced with the ability of UPy dimers to readily dissociate and exchange with water. The tensile strength and tensile toughness of the GO nacre-like film increased by up to 470% and 1100% and the maximum strain by a factor of ~2, for the film with the highest UPy content. These improvements are achieved through a mechanism of extension and unfolding of the linear chain of six carbon atoms in UPy, enhancing strain under tensile loading permitting the platelets to slide more before failure. This work highlights the impact of enhanced interlayer interactions via hydrogen bonding in producing polymer-free nacre-like films.

Item Type:	Journal Article
Subjects:	T Technology > TA Engineering (General). Civil engineering (General) T Technology > TJ Mechanical engineering and machinery
Divisions:	Faculty of Science > Physics Faculty of Science > WMG (Formerly the Warwick Manufacturing Group)
Library of Congress Subject Headings (LCSH):	Graphene , Graphene -- Industrial applications, Graphene -- Oxidation, Graphene -- Mechanical properties, Vacuum technology
Journal or Publication Title:	ACS Applied Nano Materials
Publisher:	ACS
ISSN:	2574-0970
Official Date:	5 June 2020
Dates:	Date Event 5 June 2020 Published
Date of first compliant deposit:	9 June 2020
DOI:	10.1021/acsanm.0c01488
Status:	Peer Reviewed
Publication Status:	In Press
Publisher Statement:	This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Nano Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://dx.doi.org/10.1021/acsanm.0c01488
Access rights to Published version:	Restricted or Subscription Access
RIOXX Funder/Project Grant:	Project/Grant ID RIOXX Funder Name Funder ID EP/L015307/1 [EPSRC] Engineering and Physical Sciences Research Council http://dx.doi.org/10.13039/501100000266 UNSPECIFIED Tata Motors https://lccn.loc.gov/n2010043843 EP/M028186/1 [EPSRC] Engineering and Physical Sciences Research Council http://dx.doi.org/10.13039/501100000266 EP/K024418/1 [EPSRC] Engineering and Physical Sciences Research Council http://dx.doi.org/10.13039/501100000266 UNSPECIFIED Advantage West Midlands http://dx.doi.org/10.13039/100014381 UNSPECIFIED [ERDF] European Regional Development Fund http://dx.doi.org/10.13039/501100008530

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